| 1. |
- Agostini, Marco, 1987, et al.
(författare)
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Designing a Safe Electrolyte Enabling Long‐Life Li/S Batteries
- 2019
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 12:18, s. 4176-4184
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Tidskriftsartikel (refereegranskat)abstract
- Lithium–sulfur (Li/S) batteries suffer from “shuttle” reactions in which soluble polysulfide species continuously migrate to and from the Li metal anode. As a consequence, the loss of active material and reactions at the surface of Li limit the practical applications of Li/S batteries. LiNO3 has been proposed as an electrolyte additive to reduce the shuttle reactions by aiding the formation of a stable solid electrolyte interphase (SEI) at the Li metal, limiting polysulfide shuttling. However, LiNO3 is continuously consumed during cycling, especially at low current rates. Therefore, the Li/S battery cycle life is limited by the LiNO3 concentration in the electrolyte. In this work, an ionic liquid (IL) [N-methyl-(n-butyl)pyrrolidinium bis(trifluoromethylsulfonyl)imide] was used as an additive to enable longer cycle life of Li/S batteries. By tuning the IL concentration, an enhanced stability of the SEI and lower flammability of the solutions were demonstrated, that is, higher safety of the battery. The Li/S cell built with a high sulfur mass loading (4 mg cm−2) and containing the IL-based electrolyte demonstrated a stable capacity of 600 mAh g−1 for more than double the number of cycles of a cell containing LiNO3 additive.
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| 2. |
- Brige, Amandine, et al.
(författare)
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A comparative study of hydroxyethylcellulose-based solid polymer electrolytes for solid state Zn batteries
- 2023
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Ingår i: NANO SELECT. - : Wiley. - 2688-4011. ; 4:1, s. 102-111
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Tidskriftsartikel (refereegranskat)abstract
- Rechargeable zinc metal batteries are greener and safer alternative to lithium batteries, but they suffer from poor reversibility due to growth of zinc dendrites and water splitting reactions of aqueous electrolytes. One strategy to overcome these drawbacks is replacing aqueous electrolyte with solid polymer electrolyte (SPE). In this work, we examine the possibility of fabricating solid electrolyte from a bio-based polymer, hydroxyethylcellulose (HEC), with the aim to further increase the sustainability of zinc batteries. Various types of zinc salts, drying procedures and the salt concentrations are investigated for their impact on the ionic conductivity, structure, and phase behavior of as-prepared polymer electrolytes. It is found that HEC has a good film-forming ability compared with commonly used poly(ethylene oxide) but its low salt-dissociation capability leads to an ionic conductivity of 10(-6) S cm(-1) even at the elevated temperature of 110 degrees C, hindering the possibility of solely utilizing HEC as matrix of solid electrolyte. Our results suggest that introducing a new polymer with higher salt-dissociation capability or lower glass transition temperature into the HEC matrix can be a reliable way to build solid polymer electrolytes with sufficient ionic conductivity and good mechanical property for future zinc batteries.
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| 3. |
- Calcagno, Giulio, 1990, et al.
(författare)
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Effect of Nitrogen Doping on the Performance of Mesoporous CMK-8 Carbon Anodes for Li-Ion Batteries
- 2020
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Ingår i: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:19
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Tidskriftsartikel (refereegranskat)abstract
- Designing carbonaceous materials with heightened attention to the structural properties such as porosity, and to the functionalization of the surface, is a growing topic in the lithium-ion batteries (LIBs) field. Using a mesoporous silica KIT-6 hard template, mesoporous carbons belonging to the OMCs (ordered mesoporous carbons) family, namely 3D cubic CMK-8 and N-CMK-8 were synthesized and thoroughly structurally characterized. XPS analysis confirmed the successful introduction of nitrogen, highlighting the nature of the different nitrogen atoms incorporated in the structure. The work aims at evaluating the electrochemical performance of N-doped ordered mesoporous carbons as an anode in LIBs, underlining the effect of the nitrogen functionalization. The N-CMK-8 electrode reveals higher reversible capacity, better cycling stability, and rate capability, as compared to the CMK-8 electrode. Coupling the 3D channel network with the functional N-doping increased the reversible capacity to similar to 1000 mAh center dot g(-1) for the N-CMK-8 from similar to 450 mAh center dot g(-1) for the undoped CMK-8 electrode. A full Li-ion cell was built using N-CMK-8 as an anode, commercial LiFePO4, a cathode, and LP30 commercial electrolyte, showing stable performance for 100 cycles. The combination of nitrogen functionalization and ordered porosity is promising for the development of high performing functional anodes.
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| 4. |
- Chen, Yaqi, et al.
(författare)
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Insight into the Extreme Side Reaction between LiNi0.5Co0.2Mn0.3O2 and Li1.3Al0.3Ti1.7(PO4)3 during Cosintering for All-Solid-State Batteries
- 2023
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Ingår i: Chemistry of Materials. - 1520-5002 .- 0897-4756. ; 35:22, s. 9647-9656
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Tidskriftsartikel (refereegranskat)abstract
- All-solid-sate batteries (ASSBs) with a NASICON-type solid-state electrolyte (SSE) of Li1.3Al0.3Ti1.7(PO4)3 (LATP) can be accepted as a promising candidate to significantly improve safety and energy density due to their high oxidation potential and high ionic conductivity. However, thermodynamic instability between the cathode and LATP is scarcely investigated during cosintering preparation for the integrated configuration of ASSBs. Herein, the structural compatibility between commercially layered LiNi0.5Co0.2Mn0.3O2 (NCM523) and LATP SSE was systematically investigated by cosintering at 600 °C. It is noticeable that an extreme side reaction between Li from NCM523 and phosphate from LATP happens during its cosintering process, leading to a severe phase transition from a layered to a spinel structure with high Li/Ni mixing. Consequently, the capacity of NCM523 is lost during the preparation of the NCM523-LATP composite cathode. Based on this, we suggested that the interface modification of the NCM523/LATP interface is valued significantly to inhibit this extreme side reaction, quickening the application of LATP-based ASSBs.
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| 5. |
- Chen, Yaqi, et al.
(författare)
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Two Birds with One Stone: Using Indium Oxide Surficial Modification to Tune Inner Helmholtz Plane and Regulate Nucleation for Dendrite-free Lithium Anode
- 2022
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Ingår i: Small Methods. - : Wiley. - 2366-9608. ; 6:5
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Tidskriftsartikel (refereegranskat)abstract
- Lithium metal has been considered as the most promising anode material due to its distinguished specific capacity of 3860 mAh g–1 and the lowest reduction potential of -3.04 V versus the Standard Hydrogen Electrode. However, the practicalization of Li-metal batteries (LMBs) is still challenged by the dendritic growth of Li during cycling, which is governed by the surface properties of the electrodepositing substrate. Herein, a surface modification with indium oxide on the copper current collector via magnetron sputtering, which can be spontaneously lithiated to form a composite of lithium indium oxide and Li-In alloy, is proposed. Thus, the growth of Li dendrites is effectively suppressed via regulating the inner Helmholtz plane modified with LiInO2 to foster the desolvation of Li-ion and induce the nucleation of Li-metal in two-dimensions through electro-crystallization with Li-In alloy. Using the In2O3 modification, the Li-metal anode exhibits outstanding cyclic stability, and LMBs with lithium cobalt oxide cathode present excellent capacity retention (above 80% over 600 cycles). Enlightening, the scalable magnetron sputtering method reported here paves a novel way to accelerate the practical application of the Li anode in LMBs to pursue higher energy density.
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| 6. |
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| 7. |
- Jiao, Xingxing, et al.
(författare)
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Crumpled Nitrogen-Doped Graphene-Wrapped Phosphorus Composite as a Promising Anode for Lithium-Ion Batteries
- 2019
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Ingår i: ACS Applied Materials & Interfaces. - : American Chemical Society (ACS). - 1944-8252 .- 1944-8244. ; 11:34, s. 30858-30864
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Tidskriftsartikel (refereegranskat)abstract
- Red phosphorus (P) has recently gained wide attention because of the high theoretical capacity of 2596 mA h/g, which has been regarded as promising anode material for lithium-ion batteries (LIBs). However, the actual application of red P in LIBs is hampered by the huge expansion of volume and low electronic conductivity. Herein, we design a kind of red phosphorus/crumpled nitrogen-doped graphene (P/CNG) nanocomposites with high capacity density and great rate performance as anode material for LIBs. This anode material was rationally fabricated through the scalable ball-milling method. The nanocomposite structure of P/CNG improves the electron conductivity and alleviates volume change of raw red P because of the three-dimension (3D) framework, massive defects and active sites of CNG sheets. As expected, the P/CNG composite shows excellent electrochemical performances, including high capacity (2522.6 mA h/g at 130 mA/g), remarkable rate capability (1340.5 mA h/g at 3900 mA/g), and great cyclability (1470.1 mA h/g at 1300 mA/g for 300 cycles). This work may provide a broad prospect for a great rate performance of P-based anode material for LIBs.
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| 8. |
- Jiao, Xingxing, et al.
(författare)
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Electro-chemo-mechanical failure of solid-state electrolyte caused from intergranular or transgranular damage propagation in polycrystalline aggregates
- 2024
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Ingår i: Acta Materialia. - 1359-6454. ; 265
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Tidskriftsartikel (refereegranskat)abstract
- Electro-chemo-mechanical failure of solid-state electrolytes (SEs) caused by the internal growth of lithium dendrites significantly impedes the application of solid-state batteries under high applied current density. The grain boundary is usually the key to the mechanical properties of polycrystalline ceramic SEs. Here, strength and width of grain boundary in SEs that are exampled by garnet-type Li7La3Zr2O12 are evaluated under the deposition of lithium by visualizing the stress field, damage accumulation and crack propagation. The enhancement of grain boundary strength triggers a dramatic increase stress when the ratio of tensile strength between grain boundary and grain (λ) is lower than 0.9. With the variation of λ, three damage processes are revealed as intergranular-damage, inter/transgranular-damage and transgranular-damage, leading to different propagation of cracks and the transformation of intergranular failure to transgranular failure. Furthermore, the width of the grain boundary is found to induce more transgranular-damage with its widening. A critical value of grain boundary width for the formation of displacement is obtained under various strengths, as δ = 21 nm for λ = 0.2, δ = 25 nm for λ = 0.5 and δ = 31 nm for λ = 0.9. The findings in this work indicate the coupling effect of grain boundary width and strength on the failure of SEs, providing an insightful perspective for the future design of solid-state batteries.
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| 9. |
- Jiao, Xingxing, et al.
(författare)
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Grain size and grain boundary strength: Dominative role in electro-chemo-mechanical failure of polycrystalline solid-state electrolytes
- 2024
-
Ingår i: Energy Storage Materials. - 2405-8297. ; 65
-
Tidskriftsartikel (refereegranskat)abstract
- Solid-state batteries with lithium metal anode have been accepted extensively as the competitive option to fulfill the upping requirement for safe and efficient energy devices. Nevertheless, its wide-ranging application has been impeded by the failure of solid-state electrolyte (SSE) induced by development of lithium (Li) filament. Based on the nature of polycrystalline ceramic SSE with varying grain size and boundary strength, the constitutive equation coupled with electrochemical kinetics was applied to picture the propagation of damage and corresponding disintegration caused by the development of Li filament. Based on the results, we found that the stress generated along with the growth of Li filament spreads away via the opening and sliding of grain boundary. Thus, damage occurs along grain boundaries, of which propagation behavior and damage level are controlled by grain size. Especially, over-refinement and under-refinement of grains of SSE can cause flocculent damage with inordinate damage degree and accelerate the failure time of SSE, respectively. On the other hand, the failure time is powerfully prolongated through strengthening the grain boundary of SSE. Eventually, grain size of 0.2 μm and tensile strength of grain boundary of 0.8-time-of-grain are posted as the threshold to realize the postponed failure of NASICON-based SSE. Inspiringly, electro-chemo-mechanical model in this contribution is generally applicable to other type of ceramic SSE to reveal the failure process and provide the design guideline, fostering the improvement of solid-state batteries.
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| 10. |
- Jiao, Xingxing, et al.
(författare)
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Highly Energy-Dissipative, Fast Self-Healing Binder for Stable Si Anode in Lithium-Ion Batteries
- 2021
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 31:3
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Tidskriftsartikel (refereegranskat)abstract
- A double-wrapped binder has been rationally designed with high Young's modulus polyacrylic acid (PAA) inside and low Young's modulus bifunctional polyurethane (BFPU) outside to address the large inner stress of silicon anode with drastic volume changes during cycling. Harnessing the "hard to soft" gradient distribution strategy, the rigid PAA acts as a protective layer to dissipate the inner stress first during lithiation, while the elastic binder BFPU serves as a buffer layer to disperse residual stress, and thus avoids structural damage of rigid PAA. Moreover, the introduction of BFPU with fast self-healing ability can dynamically recover the microcracks arising from large stress, further ensuring the integrity of silicon anode. This multifunctional binder with smart design of double-wrapped structure provides enlightenment on enlarging the cycling life of high-energy-density lithium-ion batteries that suffer enormous volume change during the cycling process.
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| 11. |
- Jiao, Xingxing, et al.
(författare)
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Insight of electro-chemo-mechanical process inside integrated configuration of composite cathode for solid-state batteries
- 2023
-
Ingår i: Energy Storage Materials. - 2405-8297. ; 61
-
Tidskriftsartikel (refereegranskat)abstract
- The complicated electro-chemo-mechanical process that occurs inside the composite cathode for solid-state batteries (SSBs), is of first importance to be insighted for the development of SSBs to seek higher energy density. Herein, exampled with layered transition-metal oxide of LiNixCoyMn1-x-yO2 (NCM), an electro-chemo-mechanical model containing electrochemical kinetics, finite-strain constitutive model and cohesive zone model was built to uncover the impact of ionic conductivity and Young's modulus (E) of solid-state electrolyte (SE) on the electro-chemo-mechanical process inside composite cathode and the intergranular failure of single cathode particle. The intergranular failure of NCM particles is powerfully determined by the Young's modulus of SE and the primary particle size, which is postponed by the coarse-primary NCM with soft SE of E=∼2 GPa. Compared with Young's modulus, increasing the ionic conductivity can uniform the distribution of both Li-ion and stress in the whole composite NCM cathode, realizing improved electrochemical performance with larger normalized capacity and lower the interfacial impendence. Hence, high-adequate ionic conductivity of 5 × 10−4 S cm−1 and soft mechanical property of E=∼2 GPa can be proposed as the guideline of SE for great electrochemical performance with prolongated lifespan of composite NCM cathode, paving an avenue to foster the application of SSBs.
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| 12. |
- Jiao, Xingxing, et al.
(författare)
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Morphology evolution of electrodeposited lithium on metal substrates
- 2023
-
Ingår i: Energy Storage Materials. - 2405-8297. ; 61
-
Tidskriftsartikel (refereegranskat)abstract
- Lithium (Li) metal is deemed to be the high-energy-density anode material for next generation batteries, but its practical application is impeded by the uneven electrodeposition during charge of battery, which leads to the low Coulombic efficiency and potential safety issue. Here, multiscale modeling is fabricated to understand the morphology evolution of Li during electrodeposition process, from the self-diffusion of Li adatoms on electrode surface, to the nucleation process, and to the formation of Li microstructures, revealing the correlation between final morphology and deposition substrates. Energy batteries and self-diffusion of Li adatom on various substrates (lithium, copper, nickel, magnesium, and silver) result in the different nucleation size, which is calculated by kinetic Monte Carlo simulation based on classical nucleation theory. Formation of Li substructures that are grown from Li nuclei, is revealed by phase field modeling coupled with cellular automaton method. Our results show that larger Li nuclei is obtained under faster self-diffusion of Li adatom, leading to the low aspect ratio of Li substructures and the subsequent morphology evolution of electrodeposited Li. Furthermore, the electrodeposition of Li is strongly regulated by the selection of substrates, giving the practical guideline of anode design in rechargeable Li metal batteries. It is worthy to mention that this method to investigate the electro-crystallization process involving nucleation and growth can be transplanted to the other metallic anode, such as sodium, potassium, zinc, magnesium, calcium and the like.
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| 13. |
- Jiao, Xingxing, et al.
(författare)
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Multi-Physical Field Simulation: A Powerful Tool for Accelerating Exploration of High-Energy-Density Rechargeable Lithium Batteries
- 2023
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Ingår i: Advanced Energy Materials. - 1614-6840 .- 1614-6832. ; In Press
-
Forskningsöversikt (refereegranskat)abstract
- To meet the booming demand of high-energy-density battery systems for modern power applications, various prototypes of rechargeable batteries, especially lithium metal batteries with ultrahigh theoretical capacity, have been intensively explored, which are intimated with new chemistries, novel materials and rationally designed configurations. What happens inside the batteries is associated with the interaction of multi-physical field, rather than the result of the evolution of a single physical field, such as concentration field, electric field, stress field, morphological evolution, etc. In this review, multi-physical field simulation with a relatively wide length and timescale is focused as formidable tool to deepen the insight of electrodeposition mechanism of Li metal and the electro-chemo-mechanical failure of solid-state electrolytes based on Butler-Volmer electrochemical kinetics and solid mechanics, which can promote the future development of state-of-the-art Li metal batteries with satisfied energy density as well as lifespan.
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| 14. |
- Jiao, Xingxing, et al.
(författare)
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Viability of all-solid-state lithium metal battery coupled with oxide solid-state electrolyte and high-capacity cathode
- 2024
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Ingår i: Journal of Energy Chemistry. - 2095-4956. ; 91, s. 122-131
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Tidskriftsartikel (refereegranskat)abstract
- Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g−1 and oxide-based ceramic solid-state electrolytes (SE), e.g., garnet-type Li7La3Zr2O12 (LLZO), all-state-state lithium metal batteries (ASLMBs) have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety. However, its applications are still challenged by plenty of technical and scientific issues. In this contribution, the co-sintering temperature at 500 °C is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi0.5Co0.2Mn0.3O2 (NCM). On the other hand, it tends to form weaker grain boundary (GB) inside polycrystalline LLZO at inadequate sintering temperature for LLZO, which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE. Therefore, increasing the strength of GB, refining the grain to 0.4 μm, and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB. Moreover, the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.
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| 15. |
- Kang, Hyokyeong, et al.
(författare)
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Relaxation of Stress Propagation in Alloying-Type Sn Anodes for K-Ion Batteries
- 2024
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Ingår i: Small Methods. - 2366-9608. ; 8:1
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Tidskriftsartikel (refereegranskat)abstract
- Alloying-type metallic tin is perceived as a potential anode material for K-ion batteries owing to its high theoretical capacity and reasonable working potential. However, pure Sn still face intractable issues of inferior K+ storage capability owing to the mechanical degradation of electrode against large volume changes and formation of intermediary insulating phases K4Sn9 and KSn during alloying reaction. Herein, the TiC/C–carbon nanotubes (CNTs) is prepared as an effective buffer matrix and composited with Sn particles (Sn–TiC/C–CNTs) through the high-energy ball-milling method. Owing to the conductive and rigid properties, the TiC/C–CNTs matrix enhances the electrical conductivity as well as mechanical integrity of Sn in the composite material and thus ultimately contributes to performance supremacy in terms of electrochemical K+ storage properties. During potassiation process, the TiC/C–CNTs matrix not only dissipates the internal stress toward random radial orientations within the Sn particle but also provides electrical pathways for the intermediate insulating phases; this tends to reduce microcracking and prevent considerable electrode degradation.
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| 16. |
- Lee, Suyeong, et al.
(författare)
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High-Energy and Long-Lifespan Potassium–Sulfur Batteries Enabled by Concentrated Electrolyte
- 2022
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 32:46
-
Tidskriftsartikel (refereegranskat)abstract
- Potassium–sulfur (K–S) batteries are emerging as low-cost and high-capacity energy-storage technology. However, conventional K–S batteries suffer from two critical issues that have not yet been successfully resolved: the dissolution of potassium polysulfides (KPS) into the liquid electrolyte and the formation of K dendrites on the K metal anode, which lead to inadequate cycling efficiencies with a low reversible capacity. Herein, a high-capacity and long cycle-life K–S battery consisting of a highly concentrated electrolyte (HCE) (4.34 mol kg−1 potassium bis(fluorosulfonyl)imide in a 1,2-Dimethoxyethane) and a sulfurized polyacrylonitrile (SPAN) cathode is presented The application of a HCE efficiently suppresses the dendritic growth of K, as evidenced by operando optical imaging and phase field modeling, owing to the reduced K-ion depletion on the electrode surface and a uniform Faradaic current density over the K metal anode surface. Additionally, because S is covalently bonded to the C backbone of PAN in the SPAN structure, the SPAN cathode inhibits the dissolution of KPS. These features generate synergy that the proposed K–S battery can provide a practical areal capacity of 2.5 mAh cm−2 and unprecedented lifetimes with high Coulombic efficiencies over 700 cycles.
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| 17. |
- Lee, Suyeong, et al.
(författare)
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Recent developments and future challenges in designing rechargeable potassium-sulfur and potassium-selenium batteries
- 2020
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Ingår i: Energies. - : MDPI AG. - 1996-1073 .- 1996-1073. ; 13:11
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Tidskriftsartikel (refereegranskat)abstract
- The use of chalcogenide elements, such as sulfur (S) and selenium (Se), as cathode materials in rechargeable lithium (Li) and sodium (Na) batteries has been extensively investigated. Similar to Li and Na systems, rechargeable potassium-sulfur (K-S) and potassium-selenium (K-Se) batteries have recently attracted substantial interest because of the abundance of K and low associated costs. However, K-S and K-Se battery technologies are in their infancy because K possesses overactive chemical properties compared to Li and Na and the electrochemical mechanisms of such batteries are not fully understood. This paper summarizes current research trends and challenges with regard to K-S and K-Se batteries and reviews the associated fundamental science, key technological developments, and scientific challenges to evaluate the potential use of these batteries and finally determine effective pathways for their practical development.
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| 18. |
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| 19. |
- Li, Shijia, et al.
(författare)
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Textured Na 2 V 6 O 16 ·3H 2 O Cathode Tuned via Crystal Engineering Endows Aqueous Zn-Ion Batteries with High Rate Capability and Adequate Lifespan
- 2022
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Ingår i: ACS Energy Letters. - : American Chemical Society (ACS). - 2380-8195. ; 7:11, s. 3770-3779
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Tidskriftsartikel (refereegranskat)abstract
- Aqueous zinc-ion batteries (ZIBs) play a vital role in large-scale energy storage for smart grids due to their environmental friendliness, safety, and low cost. Unfortunately, the application of ZIBs has been challenged by the relatively low capacity of cathode materials, especially at higher rates, which originates from the sluggish diffusion of Zn ions. Herein, a crystal engineering strategy is explored for using bernesite, Na2V6O16·3H2O (NVO), for regulating the diffusion-preferable texture, which was beneficial for fostering Zn ions' diffusion and thus guaranteeing a uniform concentration inside the cathode. An enlarged capacity at a higher rate was obtained, delivering a capacity of 156.9 mAh g-1 at the ultra-high current density of 20 A g-1, of which 140.6 mAh g-1 remained after 5000 cycles. The use of crystal engineering to regulate the texture of cathode materials paves the way to boost the application of NVO in aqueous ZIBs, which could be translated to design state-of-the-art cathodes for other battery systems.
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| 20. |
- Liu, Qiao, et al.
(författare)
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Enhanced ionic conductivity and interface stability of hybrid solid-state polymer electrolyte for rechargeable lithium metal batteries
- 2019
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Ingår i: Energy Storage Materials. - : Elsevier BV. - 2405-8297. ; 23, s. 105-111
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Tidskriftsartikel (refereegranskat)abstract
- Compared to conventional organic liquid electrolyte, solid-state polymer electrolytes are extensively considered as an alternative candidate for next generation high-energy batteries because of their high safety, non-leakage and electrochemical stability with the metallic lithium (Li) anode. However, solid-state polymer electrolytes generally show low ionic conductivity and high interfacial impedance to electrodes. Here we report a hybrid solid-state electrolyte, presenting an ultra-high ionic conductivity of 3.27 mS cm −1 at room temperature, a wide electrochemical stability window of 4.9 V, and non-flammability. This electrolyte consists of a polymer blend matrix (polyethylene oxide and poly (vinylidene fluoride-co-hexafluoropropylene)), Li + conductive ceramic filler (Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 ) and a solvate ionic liquid (LiFSI in tetra ethylene glycol dimethyl ether, 1:1 in molar ratio) as plasticizer. The introduction of the solvate ionic liquid to the solid-state electrolyte not only improves its ionic conductivity but also remarkably enhances the stability of the interface with Li anode. When applied in Li metal batteries, a Li|Li symmetric cell can operate stably over 800 h with a minimal polarization of 25 mV and a full Li|LiFePO 4 cell delivers a high specific capacity of 158 mAh g −1 after 100 cycles at room temperature.
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| 21. |
- Liu, Yangyang, et al.
(författare)
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Electro-Chemo-Mechanical Modeling of Artificial Solid Electrolyte Interphase to Enable Uniform Electrodeposition of Lithium Metal Anodes
- 2022
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Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 12:9
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Tidskriftsartikel (refereegranskat)abstract
- Nonuniform electrodeposition of lithium during charging processes is the key issue hindering development of rechargeable Li metal batteries. This deposition process is largely controlled by the solid electrolyte interphase (SEI) on the metal surface and the design of artificial SEIs is an essential pathway to regulate electrodeposition of Li. In this work, an electro-chemo-mechanical model is built and implemented in a phase-field modelling to understand the correlation between the physical properties of artificial SEIs and deposition of Li. The results show that improving ionic conductivity of the SEI above a critical level can mitigate stress concentration and preferred deposition of Li. In addition, the mechanical strength of the SEI is found to also mitigate non-uniform deposition and influence electrochemical kinetics, with a Young's modulus around 4.0 GPa being a threshold value for even deposition of Li. By comparison of the results to experimental results for artificial SEIs it is clear that the most important direction for future work is to improve the ionic conductivity without compromising mechanical strength. In addition, the findings and methodology presented here not only provide detailed guidelines for design of artificial SEI on Li-metal anodes but also pave the way to explore strategies for regulating deposition of other metal anodes.
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| 22. |
- Liu, Yangyang, et al.
(författare)
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Insight into the Critical Role of Exchange Current Density on Electrodeposition Behavior of Lithium Metal
- 2021
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Ingår i: Advanced Science. - : Wiley. - 2198-3844 .- 2198-3844. ; 8:5
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Tidskriftsartikel (refereegranskat)abstract
- Due to an ultrahigh theoretical specific capacity of 3860 mAh g−1, lithium (Li) is regarded as the ultimate anode for high-energy-density batteries. However, the practical application of Li metal anode is hindered by safety concerns and low Coulombic efficiency both of which are resulted fromunavoidable dendrite growth during electrodeposition. This study focuses on a critical parameter for electrodeposition, the exchange current density, which has attracted only little attention in research on Li metal batteries. A phase-field model is presented to show the effect of exchange current density on electrodeposition behavior of Li. The results show that a uniform distribution of cathodic current density, hence uniform electrodeposition, on electrode is obtained with lower exchange current density. Furthermore, it is demonstrated that lower exchange current density contributes to form a larger critical radius of nucleation in the initial electrocrystallization that results in a dense deposition of Li, which is a foundation for improved Coulombic efficiency and dendrite-free morphology. The findings not only pave the way to practical rechargeable Li metal batteries but can also be translated to the design of stable metal anodes, e.g., for sodium (Na), magnesium (Mg), and zinc (Zn) batteries.
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| 23. |
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| 24. |
- Liu, Yangyang, et al.
(författare)
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Promoted rate and cycling capability of Li–S batteries enabled by targeted selection of co-solvent for the electrolyte
- 2020
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Ingår i: Energy Storage Materials. - : Elsevier BV. - 2405-8297. ; 25, s. 131-136
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Tidskriftsartikel (refereegranskat)abstract
- Lithium sulfur (Li–S) batteries are considered as promising candidates for high-energy-density battery systems owing to the high theoretical capacity of sulfur (1675 mAh g−1) and low cost of raw materials. However, their practical application is hampered by low rate capability and rapid degradation of capacity, arising from the passivation of the cathode by lithium sulfides (Li2S2/Li2S) deposited during discharge and low interfacial stability of the Li anode. Herein, we report on a comprehensive strategy to select co-solvent to the electrolyte to regulate the deposition of lithium sulfides during charge-discharge process. We show that addition of a co-solvent with high solubility, and strong interaction with Li2S to a conventional electrolyte effectively mitigates the formation of a passivating layer on the sulfur cathode and dramatically improves the interfacial stability of the Li anode. We demonstrate that Sulfolane (SL) has these properties and that a Li–S cell with an electrolyte containing 6 vol% SL exhibits outstanding cyclic performance (0.083% decay per cycle) and rate capability (capacity density of 765 mAh g−1 at rate of 1.0C). Thus, we provide a facile strategy for the selection of co-solvent for improved performance of Li–S batteries, realizing their practical application for high-energy-density battery systems.
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| 25. |
- Liu, Yangyang, et al.
(författare)
-
Role of Interfacial Defects on Electro–Chemo–Mechanical Failure of Solid-State Electrolyte
- 2023
-
Ingår i: Advanced Materials. - 0935-9648 .- 1521-4095. ; 35:24
-
Tidskriftsartikel (refereegranskat)abstract
- High-stress field generated by electroplating of lithium (Li) in pre-existing defects is the main reason for mechanical failure of solid-state electrolyte because it drives crack propagation in electrolyte, followed by Li filament growth inside and even internal short-circuit if the filament reaches another electrode. To understand the role of interfacial defects on mechanical failure of solid-state electrolyte, an electro–chemo–mechanical model is built to visualize distribution of stress, relative damage, and crack formation during electrochemical plating of Li in defects. Geometry of interfacial defect is found as dominating factor for concentration of local stress field while semi-sphere defect delivers less accumulation of damage at initial stage and the longest failure time for disintegration of electrolyte. Aspect ratio, as a key geometric parameter of defect, is investigated to reveal its impact on failure of electrolyte. Pyramidic defect with low aspect ratio of 0.2–0.5 shows branched region of damage near interface, probably causing surface pulverization of solid-state electrolyte, whereas high aspect ratio over 3.0 will trigger accumulation of damage in bulk electrolyte. The correction between interfacial defect and electro–chemo–mechanical failure of solid-state electrolyte is expected to provide insightful guidelines for interface design in high-power-density solid-state Li metal batteries.
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| 26. |
- Liu, Yangyang, et al.
(författare)
-
Stable Li metal anode by crystallographically oriented plating through in-situ surface doping
- 2020
-
Ingår i: Science China Materials. - : Springer Science and Business Media LLC. - 2199-4501 .- 2095-8226. ; 63:6, s. 1036-1045
-
Tidskriftsartikel (refereegranskat)abstract
- Lithium (Li) metal is regarded as the holy grail anode material for high-energy-density batteries owing to its ultrahigh theoretical specific capacity. However, its practical application is severely hindered by the high reactivity of metallic Li against the commonly used electrolytes and uncontrolled growth of mossy/dendritic Li. Different from widely-used approaches of optimization of the electrolyte and/or interfacial engineering, here, we report a strategy of in-situ cerium (Ce) doping of Li metal to promote the preferential plating along the [200] direction and remarkably decreased surface energy of metallic Li. The in-situ Ce-doped Li shows a significantly reduced reactivity towards a standard electrolyte and, uniform and dendrite-free morphology after plating/stripping, as demonstrated by spectroscopic, morphological and electrochemical characterizations. In symmetric half cells, the in-situ Ce-doped Li shows a low corrosion current density against the electrolyte and drastically improved cycling even at a lean electrolyte condition. Furthermore, we show that the stable Li LiCoO2 full cells with improved coulombic efficiency and cycle life are also achieved using the Ce-doped Li metal anode. This work provides an inspiring approach to bring Li metal towards practical application in high energy-density batteries.
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| 27. |
- Lundin, Filippa, 1992, et al.
(författare)
-
Ion Dynamics and Nanostructures of Diluted Ionic Liquid Electrolytes
- 2022
-
Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 126:38, s. 16262-16271
-
Tidskriftsartikel (refereegranskat)abstract
- Diluted ionic liquid electrolytes are promising candidates in next-generation batteries enabling the implementation of lithium metal anodes. The diluent should fully mix with the ionic liquid while not interacting with the Li ions to preserve the ionic liquid character, which is beneficial for Li-metal electrode stability. We report on the influence of a hydrofluoroether (HFE) diluent on ion dynamics and nanostructure of an ionic liquid electrolyte. We show that the ionic liquid and the diluent are fully miscible and that the solvation structure of the Li ions is not affected by the presence of HFE. The increase in the conductivity by the addition of the diluent is directly related to a decrease in viscosity with faster dynamics of all ionic species. However, the relative increase in mobility is considerably larger for the ionic liquid cation as a result of a preferred interaction with HFE. On the microscopic scale, more complex local non-Gaussian diffusive dynamics are found, faster than what is expected from the self-diffusion coefficient. The relative change of the dynamics with the addition of HFE on macro- and microscopic length scales correlates well, which underlines the connection between the motions probed on different length and time scales.
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| 28. |
- Nitze, Florian, 1981, et al.
(författare)
-
Sulfur-doped ordered mesoporous carbons: A stability-improving sulfur host for lithium-sulfur battery cathodes
- 2016
-
Ingår i: Journal of Power Sources. - : Elsevier BV. - 0378-7753. ; 317, s. 112-119
-
Tidskriftsartikel (refereegranskat)abstract
- We report on sulfur-functionalized ordered mesoporous carbons aimed for lithium-sulfur battery electrode applications with improved charge capacity retention. The carbons were obtained by a hard-template strategy using a mixture of furfuryl alcohol and furfuryl mercaptan. For the application as electrode material in lithium-sulfur batteries, the carbons were additionally loaded with sulfur following a traditional melt-diffusion approach. It was found that the sulfur interacts stronger with the sulfur-functionalized carbon matrix than with the non-functionalized material. Electrodes showed very high capacity in the second discharge-charge cycle amounting to approximately 1500, 1200 and 1400 mAh/g (sulfur) for carbon materials with no, medium and high degrees of sulfur functionalization, respectively. More importantly, the sulfur-functionalization of the carbon was found to increase the capacity retention after 50 discharge-charge cycles by 8 and 5% for the carbons with medium and high degrees of sulfur-functionalization, respectively, compared to carbon with no sulfur-functionalization. We attribute this significant improvement to the presence of covalently bound sulfur groups at the internal surface of the functionalized carbon providing efficient anchoring sites for catenation to the sulfur loaded into the pores of the carbons and provide experimental support for this in the form of results from cyclic voltammetry and X-ray photoelectron spectroscopy.
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| 29. |
- Oh, Gwangeon, et al.
(författare)
-
Stabilizing Layered-Type K 0.4 V 2 O 5 Cathode by K Site Substitution with Strontium for K-Ion Batteries
- 2024
-
Ingår i: Advanced Functional Materials. - 1616-3028 .- 1616-301X. ; In Press
-
Tidskriftsartikel (refereegranskat)abstract
- Developing suitable cathodes with high capacity and high power is challenging for K-ion batteries. Herein, electrochemical K-ion storage properties of the layered-type K0.4V2O5 (KVO) cathode by incorporating divalent strontium ions (Sr2+) into its crystal structure are enhanced. Divalent strontium ions (1.18 Å) are preferentially incorporated into the octahedrally coordinated K (1.38 Å) layers due to the similar ionic size compared to V4+ (0.58 Å). The introduction of 3 mmol of Sr ions in the KVO crystal improves electrical conductivity and reduces K-ion diffusion energy barriers. In addition, the strong Sr2+ and O2− interaction acts as a structural pillar, suppressing irreversible phase transition during charge–discharge process. Multi-physics simulations clearly confirm that the K0.34Sr0.03V2O5 (KS3VO) cathode exhibits a more uniform K-ion distribution and enhanced reactions of K-ions compared to the KVO cathode at various depths of discharge. As a result, the KS3VO cathode demonstrates improved reversible capacity, cycling stability, and power capability over the KVO cathode in a K-ion cell. Synchrotron X-ray analysis reveals how Sr substitution enhances the electrochemical K-ion storage properties of the KS3VO cathode. In addition, the KS3VO cathode exhibits superior thermal stability and cycling stability in a full cell coupled with a hard carbon anode compared to the KVO cathode.
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| 30. |
- Park, Jimin, et al.
(författare)
-
A Dual-Functional Electrolyte Additive for High-Performance Potassium Metal Batteries
- 2023
-
Ingår i: Advanced Functional Materials. - 1616-3028 .- 1616-301X. ; 33:48
-
Tidskriftsartikel (refereegranskat)abstract
- Potassium metal batteries (KMBs) coupled with layered transition metal oxides as cathode materials are a promising energy−storage technology owing to low cost and high capacity. However, uncontrollable dendritic growth in the K−metal anode and chemical reactivity of the layered transition metal oxide cathode against the electrolyte solution cause KMBs to suffer from low Coulombic efficiency, rapid capacity fading, and critical safety issues. In this study, an electrolyte engineering strategy is introduced by introducing adiponitrile (ADN) as a dual−functional electrolyte additive containing an electron−rich nitrile group (C≡N) in its molecule structure. Thus, the addition of 1 wt.% ADN can alter the chemical properties of the electrolyte solution, thereby improving the anode−electrolyte and cathode−electrolyte interfacial stabilities in KMBs. The formation of a potassiophilic compound with C≡N in the solid electrolyte interphase layer can guide the uniform electrodeposition of K and suppress the dendritic growth in the K−metal. Moreover, C≡N forms a strong coordination bond with the oxidized transition metal, leading the reversible redox reactions by mitigating the undesirable disproportionation reaction and improving the thermal stability of the layered transition metal oxide cathode. Computational calculations and experimental characterizations are used to verify the role of ADN additive in enhancing the electrochemical properties of KMBs.
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| 31. |
- Park, Jimin, et al.
(författare)
-
Regulating the Solvation Structure of Electrolyte via Dual–Salt Combination for Stable Potassium Metal Batteries
- 2023
-
Ingår i: Advanced Science. - 2198-3844 .- 2198-3844. ; 10:16
-
Tidskriftsartikel (refereegranskat)abstract
- Batteries using potassium metal (K-metal) anode are considered a new type of low-cost and high-energy storage device. However, the thermodynamic instability of the K-metal anode in organic electrolyte solutions causes uncontrolled dendritic growth and parasitic reactions, leading to rapid capacity loss and low Coulombic efficiency of K-metal batteries. Herein, an advanced electrolyte comprising 1 M potassium bis(fluorosulfonyl)imide (KFSI) + 0.05 M potassium hexafluorophosphate (KPF6) dissolved in dimethoxyethane (DME) is introduced as a simple and effective strategy of regulated solvation chemistry, showing an enhanced interfacial stability of the K-metal anode. Incorporating 0.05 M KPF6 into the 1 M KFSI in DME electrolyte solution decreases the number of solvent molecules surrounding the K ion and simultaneously leads to facile K+ de-solvation. During the electrodeposition process, these unique features can lower the exchange current density between the electrolyte and K-metal anode, thereby improving the uniformity of K electrodeposition, as well as potentially suppressing dendritic growth. Even under a high current density of 4 mA cm−2, the K-metal anode in 0.05 M KPF6-containing electrolyte ensures high areal capacity and an unprecedented lifespan with stable Coulombic efficiency in both symmetrical half-cells and full-cells employing a sulfurized polyacrylonitrile cathode.
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| 32. |
- Park, Jimin, et al.
(författare)
-
Stable Solid Electrolyte Interphase for Long-Life Potassium Metal Batteries
- 2022
-
Ingår i: ACS Energy Letters. - : American Chemical Society (ACS). - 2380-8195. ; 7:1, s. 401-409
-
Tidskriftsartikel (refereegranskat)abstract
- Potassium (K) is considered to be the most suitable anode material for rechargeable K batteries because of its high theoretical capacity (686 mAh g(-1)) and low redox potential (-2.93 V vs SHE). However, uneven electrodeposition of K during cycling usually leads to the growth of dendrites, resulting in low Coulombic efficiency and compromising battery safety. Herein, we develop a strategy for stabilizing K metal through simple interface control. The conductive passivation layer can be controllably designed by a spontaneous chemical reaction when a K metal foil is kept in contact with a liquid-phase potassium-polysulfide (PPS); this guides the formation of an electronically and ionically conductive solid electrolyte interphase layer including K2S compound, enabling dense K plating with a dendrite-free morphology. Compared to the bare K metal anode, the PPS-treated K metal anode demonstrates superior cycling stability in symmetric half cells and full cells using a TiS2 cathode under practical constraints.
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| 33. |
- Rizell, Josef, 1996, et al.
(författare)
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Electrochemical Signatures of Potassium Plating and Stripping
- 2024
-
Ingår i: Journal of the Electrochemical Society. - 1945-7111 .- 0013-4651. ; 171:2
-
Tidskriftsartikel (refereegranskat)abstract
- Alkali metal anodes can enable unmatched energy densities in next generation batteries but suffer from insufficient coulombic efficiencies. To deduce details about processes taking place during galvanostatic cycling, voltage profiles are commonly analyzed, however the interpretation is not straightforward as multiple processes can occur simultaneously. Here we provide a route to disentangle and interpret features of the voltage profile in order to build a mechanistic understanding on alkali metal stripping and deposition, by investigating potassium metal deposition as a model case where processes and reactions are exaggerated due to the high reactivity of potassium. In particular, the importance of separating SEI formation and nucleation to correctly estimate the energy barrier for nucleation is demonstrated. Further, we show how the native layer formed on alkali metal foils gives rise to strong features in the voltage profile and propose forming alkali metal electrode through electrodeposition to mitigate these effects.
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| 34. |
- Rizell, Josef, 1996, et al.
(författare)
-
Neutron Reflectometry Study of Solid Electrolyte Interphase Formation in Highly Concentrated Electrolytes
- 2023
-
Ingår i: Small Structures. - : WILEY. - 2688-4062. ; 4:11
-
Tidskriftsartikel (refereegranskat)abstract
- Highly concentrated electrolytes have been found to improve the cycle life and Coulombic efficiency of lithium metal anodes, as well as to suppress dendrite growth. However, the mechanism for these improvements is not well understood. Partly, this can be linked to the difficulty of accurately characterizing the solid electrolyte interphase (SEI), known to play an important role for anode stability and stripping/plating efficiency. Herein, in situ neutron reflectometry is used to obtain information about SEI formation in a highly concentrated ether-based electrolyte. With neutron reflectometry, the thickness, scattering length density (SLD), and roughness of the SEI layer formed on a Cu working electrode are nondestructively probed. The reflectivity data point to the formation of a thin (5 nm) SEI in the highly concentrated electrolyte (salt:solvent ratio 1:2.2), while a considerably thicker (13 nm) SEI is formed in an electrolyte at lower salt concentration (salt:solvent ratio 1:13.7). Further, the SEI formed in the electrolyte with high salt concentration has a higher SLD, suggesting that the chemical composition of the SEI changes. The results from neutron reflectometry correlate well with the electrochemical data from SEI formation.
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| 35. |
- Sadd, Matthew, 1994, et al.
(författare)
-
Investigating microstructure evolution of lithium metal during plating and stripping via operando X-ray tomographic microscopy
- 2023
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 14
-
Tidskriftsartikel (refereegranskat)abstract
- Efficient lithium metal stripping and plating operation capable of maintaining electronic and ionic conductivity is crucial to develop safe lithium metal batteries. However, monitoring lithium metal microstructure evolution during cell cycling is challenging. Here, we report the development of an operando synchrotron X-ray tomographic microscopy method capable of probing in real-time the formation, growth, and dissolution of Li microstructures during the cycling of a Li||Cu cell containing a standard non-aqueous liquid electrolyte solution. The analyses of the operando X-ray tomographic microscopy measurements enable tracking the evolution of deposited Li metal as a function of time and applied current density and distinguishing the formation of electrochemically inactive Li from the active bulk of Li microstructures. Furthermore, in-depth analyses of the Li microstructures shed some light on the structural connectivity of deposited Li at different current densities as well as the formation mechanism of fast-growing fractal Li microstructures, which are ultimately responsible for cell failure.
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| 36. |
- Sadd, Matthew, 1994, et al.
(författare)
-
Polysulfide Speciation and Migration in Catholyte Lithium−Sulfur Cells
- 2022
-
Ingår i: ChemPhysChem. - : Wiley. - 1439-7641 .- 1439-4235. ; 23:4
-
Tidskriftsartikel (refereegranskat)abstract
- Semi-liquid catholyte Lithium−Sulfur (Li−S) cells have shown to be a promising path to realize high energy density energy storage devices. In general, Li−S cells rely on the conversion of elemental sulfur to soluble polysulfide species. In the case of catholyte cells, the active material is added through polysulfide species dissolved in the electrolyte. Herein, we use operando Raman spectroscopy to track the speciation and migration of polysulfides in the catholyte to shed light on the processes taking place. Combined with ex-situ surface and electrochemical analysis we show that the migration of polysulfides is central in order to maximize the performance in terms of capacity (active material utilization) as well as interphase stability on the Li-metal anode during cycling. More specifically we show that using a catholyte where the polysulfides have the dual roles of active material and conducting species, e. g. no traditional Li-salt (such as LiTFSI) is present, results in a higher mobility and faster migration of polysulfides. We also reveal how the formation of long chain polysulfides in the catholyte is delayed during charge as a result of rapid formation and migration of shorter chain species, beneficial for reaching higher capacities. However, the depletion of ionic species during the last stage of charge, due to the conversion to and precipitation of elemental sulfur on the cathode support, results in polarization of the cell before full conversion can be achieved.
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| 37. |
- Sonker, Amit Kumar, 1989, et al.
(författare)
-
Exfoliated MoS 2 Nanosheet/Cellulose Nanocrystal Flexible Composite Films as Electrodes for Zinc Batteries
- 2023
-
Ingår i: ACS Applied Nano Materials. - 2574-0970. ; 6:10, s. 8270-8278
-
Tidskriftsartikel (refereegranskat)abstract
- The study presents a more efficient way of exfoliating MoS2 in water and the exfoliated MoS2 was used in an electrode. The electrodes were prepared from exfoliated MoS2 (active material)-nanocrystalline cellulose (binder) with carbon nanotubes (electron-conducting support) and demonstrated in a zinc battery half-cell that showed a Coulombic efficiency of 90%. Successful exfoliation of MoS2 was done by sonication of bulk MoS2 with sulfated cellulose nanocrystals (CNC) for 4 h. The exfoliation was confirmed by Raman and transmission electron microscopy; interestingly, the Raman signals for exfoliated MoS2 show a blue shift for both A1g and E2g1 bands, which may be an indication of an induced lattice strain effect from the CNC on MoS2. The resulting stable water suspension showed no tendency of precipitation after 2 months of standing. The zeta potential, ζ, for sodium sulfated CNC (CNC-OSO3Na)-MoS2 in water suspension was −45 mV, whereas sulfated CNC (CNC-OSO3H)-MoS2 in water suspension had a zeta potential of −35 mV. The sodium form of sulfated CNCs displayed micelle characteristics, similar to sodium dodecyl sulfate (SDS), with a critical aggregation concentration (CAC) of 1.1 wt %. At CAC, the CNCs efficiently exfoliated MoS2, which is at a much lower concentration than has been reported for synthetic surfactants like SDS and cetyl trimethyl ammonium bromide.
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| 38. |
- Sun, Weiwei, et al.
(författare)
-
Monodispersed FeS 2 Electrocatalyst Anchored to Nitrogen-Doped Carbon Host for Lithium–Sulfur Batteries
- 2022
-
Ingår i: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 32:43
-
Tidskriftsartikel (refereegranskat)abstract
- Despite their high theoretical energy density, lithium–sulfur (Li–S) batteries are hindered by practical challenges including sluggish conversion kinetics and shuttle effect of polysulfides. Here, a nitrogen-doped continuous porous carbon (CPC) host anchoring monodispersed sub-10 nm FeS2 nanoclusters (CPC@FeS2) is reported as an efficient catalytic matrix for sulfur cathode. This host shows strong adsorption of polysulfides, promising the inhibition of polysulfide shuttle and the promoted initial stage of catalytic conversion process. Moreover, fast lithium ion (Li-ion) diffusion and accelerated solid–solid conversion kinetics of Li2S2 to Li2S on CPC@FeS2 host guarantee boosted electrochemical kinetics for conversion process of sulfur species in Li–S cell, which gives a high utilization of sulfur under practical conditions of high loading and low electrolyte/sulfur (E/S) ratio. Therefore, the surfur cathode (S/CPC@FeS2) delivers a high specific capacity of 1459 mAh g−1 at 0.1 C, a stable cycling over 900 cycles with ultralow fading rate of 0.043% per cycle, and an enhanced rate capability compared with cathode only using carbon host. Further demonstration of this cathode in Li–S pouch cell shows a practical energy density of 372 Wh kg−1 with a sulfur loading of 7.1 mg cm−2 and an E/S ratio of 4 µL mg−1.
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| 39. |
- Wu, Quan, et al.
(författare)
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Electro-Chemo-Mechanical Failure Mechanisms of Solid-State Electrolytes
- 2023
-
Ingår i: Batteries and Supercaps. - 2566-6223. ; 6:11
-
Forskningsöversikt (refereegranskat)abstract
- Solid-state lithium-metal batteries (SSLMBs) are considered as the next-generation energy storage systems due to their high theoretical energy density and safety. However, the practical deployment of SSLMBs has been impeded by the failure of solid-state electrolytes (SSEs) which is indicated by the increased impedance, elevated polarization, and capacity degradation. The failure is commonly a result of lithium (Li) dendrite growth and propagation, inactive Li generation, unstable interface formation, void and pore formation, and crack infiltration. The failure processes can be divided into electric failure, (electro)chemical failure, and mechanical failure based on the different mechanisms. The systematical understanding of SSEs failure is crucial for the development of SSEs. Therefore, this review comprehensively summarizes the details of the three SSEs failure to provide new insights for future studies, shedding light on the design of SSLMBs with high energy density, safety, and cycling stability. Failure mechanisms: This review provides a comprehensive summary of the coupled electro-chemo-mechanical failure mechanisms of solid-state electrolytes. The electric failure results from the short circuits caused by growth and propagation of Li dendrites and the capacity loss because of inactive Li formation. The formation of kinetics/thermal unstable interphase accounts for the (electro)chemical failure. Cracks infiltration and voids/pores formation lead to mechanical failure.
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| 40. |
- Xiong, Shizhao, 1985
(författare)
-
Architectural Design of Anode Materials
- 2022
-
Ingår i: ACS Symposium Series. - Washington, DC : American Chemical Society. - 1947-5918 .- 0097-6156. ; 1414, s. 133-151
-
Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Theoretical Understanding to Design a Better Solid-State Battery. Solid-state batteries have the potential to significantly improve the safety and performance of current state-of-the-art lithium-ion battery technology. They find applications in automobile and electronic industries; however, most commercial lithium-ion batteries are flammable, and their decomposition generates highly toxic gasses that can be explosive. These two volumes (1413 and 1414) provide an overview of fundamental mechanisms, current challenges, and design strategies for solid-state batteries to meet the current demands for commercialization. This volume focuses on materials, advanced batteries, and the architecture of flexible and printable batteries. These volumes should interest chemists and materials scientists working on energy challenges.
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| 41. |
- Xiong, Shizhao, 1985, et al.
(författare)
-
Design of a Multifunctional Interlayer for NASCION-Based Solid-State Li Metal Batteries
- 2020
-
Ingår i: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 30:22
-
Tidskriftsartikel (refereegranskat)abstract
- NASCION-type Li conductors have great potential to bring high capacity solid-state batteries to realization, related to its properties such as high ionic conductivity, stability under ambient conditions, wide electrochemical stability window, and inexpensive production. However, their chemical and thermal instability toward metallic lithium (Li) has severely hindered attempts to utilize Li as anode material in NASCION-based battery systems. In this work, it is shown how a tailored multifunctional interlayer between the solid electrolyte and Li anode can successfully address the interfacial issues. This interlayer is designed by creating a quasi-solid-state paste in which the functionalities of LAGP (Li1.5Al0.5Ge1.5(PO4)3) nanoparticles and an ionic liquid (IL) electrolyte are combined. In a solid-sate cell, the LAGP-IL interlayer separates the Li metal from bulk LAGP and creates a chemically stable interface with low resistance (≈5 Ω cm2) and efficiently prevents thermal runaway at elevated temperatures (300 °C). Solid-state cells designed with the interlayer can be operated at high current densities, 1 mA cm−2, and enable high rate capability with high safety. Here developed strategy provides a generic path to design interlayers for solid-state Li metal batteries.
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| 42. |
- Xiong, Shizhao, 1985, et al.
(författare)
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Lithium electrodeposition for energy storage: filling the gap between theory and experiment
- 2022
-
Ingår i: Materials Today Energy. - : Elsevier BV. - 2468-6069. ; 28
-
Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- Lithium (Li) metal has been considered a promising anode material for high-energy-density rechargeable batteries, but its utilization is impeded by the nonuniform electrodeposition during the charging process which leads to poor cycling life and safety concerns. Thus, understanding the electrodeposition mechanism of Li-metal anode is of great importance to develop practical engineering strategies for rechargeable Li-metal batteries. The electrodeposition of Li is controlled by both thermodynamic and kinetic factors, such as the solvation free energy of Li-ions, the Li nucleation, the surface diffusion of Li atom, and the strength of the interaction between Li-ion and the electrolyte anion. The scale of the whole process from the Li-ion reduction to the growth of a Li nucleus goes from sub-nanometer up to a few micrometers, which poses an outstanding challenge to both experiments and simulation. In this perspective, we discuss the top-down, the bottom-up, and the middle-way approaches to this challenge and the possible synergies between them.
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| 43. |
- Xiong, Shizhao, 1985, et al.
(författare)
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Mechanical Failure of Solid-State Electrolyte Rooted in Synergy of Interfacial and Internal Defects
- 2023
-
Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 13:14
-
Tidskriftsartikel (refereegranskat)abstract
- The mechanical failure of solid-state electrolytes induced by the growth of the lithium metal anode hinders the development of solid-state Li metal batteries with good safety and high energy density, and thus the understanding of the failure mechanism is of high importance for the application of solid-state lithium-metal batteries. Herein, a modified electro-chemo-mechanical model is built to bridge the dynamic relationship between the mechanical failure of solid-state electrolytes and the electrodeposition of lithium metal. The results, visualize evolution of local stress fields and the corresponding relative damage, and indicate that the generation of damage inside the solid-state electrolyte is rooted in a synergy of interfacial and internal defects. Compression by electrodeposited lithium inside interfacial defects and further transmission of stress inward in the electrolyte causes catastrophic damage, which is determined by the geometry of interfacial defects. Moreover, the internal defects of the solid-state electrolyte from sintering can influence the pathway of damage and work as the inner fountainhead for further damage propagation, and as such, the position and amount of the internal voids exhibit a more competitive role in the mechanical failure of solid-state electrolyte. Thus, the synergetic failure mechanism of solid-state electrolytes raised in this work provides a modeling framework to design effective strategies for state-of-the-art solid-state lithium-metal batteries.
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| 44. |
- Xiong, Shizhao, 1985, et al.
(författare)
-
Role of organic solvent addition to ionic liquid electrolytes for lithium–sulphur batteries
- 2015
-
Ingår i: RSC Advances. - : Royal Society of Chemistry (RSC). - 2046-2069.
-
Tidskriftsartikel (refereegranskat)abstract
- We investigate the role of the addition of an organic solvent to an ionic liquid electrolyte for the performance of lithium–sulphur (Li–S) batteries. We find that with a mixed electrolyte, formed by adding 10 wt% 1,3-dioxolane (DIOX) to an ionic liquid, the capacity of a Li–S cell is more than doubled, the rate capability and the cycling performance considerably improved, compared to a cell utilizing a neat ionic liquid electrolyte. The improved performance can be correlated with an enhanced ion transport, evidenced by an increased ionic conductivity and higher limiting current density, directly related to a decrease in viscosity and glass transition temperature of the mixed electrolytes. We show that this in turn is linked to a change in the local environment of the Li-ions where the organic solvent is incorporated in the coordination shell. In addition we show that the mixed electrolytes have a considerably higher thermal stability, in particular a dramatically increased flash point, and improved low temperature properties with respect to a conventional organic solvent based electrolyte currently used for Li–S batteries.
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| 45. |
- Xu, Xieyu, et al.
(författare)
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Diffusion Limited Current Density: A Watershed in Electrodeposition of Lithium Metal Anode
- 2022
-
Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 12:19
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Tidskriftsartikel (refereegranskat)abstract
- Lithium metal is considered to be a promising anode material for high-energy-density rechargeable batteries because of its high theoretical capacity and low reduction potential. Nevertheless, the practical application of Li anodes is challenged by poor cyclic performance and potential safety hazards, which are attributed to non-uniform electrodeposition of Li metal during charging. Herein, diffusion limited current density (DLCD), one of the critical fundamental parameters that govern the electrochemical reaction process, is investigated as the threshold of current density for electrodeposition of Li. The visualization of the concentration field and distribution of Faradic current density reveal how uniform electrodeposition of Li metal anodes can be obtained when the applied current density is below the DLCD of the related electrochemical system. Moreover, the electrodeposition of Li metal within broken solid electrolyte interphases preferentially occurs at the crack spots that are caused by the non-uniform electrodeposition of Li metal. This post-electrodeposition leads to more consumption of active Li when the applied current density is greater than the DLCD. Therefore, lowering the applied current density or increasing the DLCD are proposed as directions for developing advanced strategies to realize uniform electrodeposition of Li metal and stable interfaces, aiming to accelerate the practical application of state-of-the-art Li metal batteries.
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| 46. |
- Xu, Xieyu, et al.
(författare)
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Electro-Chemo-Mechanical Failure of Solid Electrolytes Induced by Growth of Internal Lithium Filaments
- 2022
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Ingår i: Advanced Materials. - : Wiley. - 0935-9648 .- 1521-4095. ; 34:49
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Tidskriftsartikel (refereegranskat)abstract
- Growth of lithium (Li) filaments within solid electrolytes, leading to mechanical degradation of the electrolyte and even short circuit of the cell under high current density, is a great barrier to commercialization of solid-state Li-metal batteries. Understanding of this electro-chemo-mechanical phenomenon is hindered by the challenge of tracking local fields inside the solid electrolyte. Here, a multiphysics simulation aiming to investigate evolution of the mechanical failure of the solid electrolyte induced by the internal growth of Li is reported. Visualization of local stress, damage, and crack propagation within the solid electrolyte enables examination of factors dominating the degradation process, including the geometry, number, and size of Li filaments and voids in the electrolyte. Relative damage induced by locally high stress is found to preferentially occur in the region of the electrolyte/Li interface having great fluctuations. A high number density of Li filaments or voids triggers integration of damage and crack networks by enhanced propagation. This model is built on coupling of mechanical and electrochemical processes for internal plating of Li, revealing evolution of multiphysical fields that can barely be captured by the state-of-the-art experimental techniques. Understanding mechanical degradation of solid electrolytes with the presence of Li filaments paves the way to design advanced solid electrolytes for future solid-state Li-metal batteries.
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| 47. |
- Xu, Xieyu, et al.
(författare)
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Role of Li-Ion Depletion on Electrode Surface: Underlying Mechanism for Electrodeposition Behavior of Lithium Metal Anode
- 2020
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Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6840 .- 1614-6832. ; 10:44
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Tidskriftsartikel (refereegranskat)abstract
- The application of lithium metal as an anode material for next generation high energy-density batteries has to overcome the major bottleneck that is the seemingly unavoidable growth of Li dendrites caused by non-uniform electrodeposition on the electrode surface. This problem must be addressed by clarifying the detailed mechanism. In this work the mass-transfer of Li-ions is investigated, a key process controlling the electrochemical reaction. By a phase field modeling approach, the Li-ion concentration and the electric fields are visualized to reveal the role of three key experimental parameters, operating temperature, Li-salt concentration in electrolyte, and applied current density, on the microstructure of deposited Li. It is shown that a rapid depletion of Li-ions on electrode surface, induced by, e.g., low operating temperature, diluted electrolyte and a high applied current density, is the underlying driving force for non-uniform electrodeposition of Li. Thus, a viable route to realize a dendrite-free Li plating process would be to mitigate the depletion of Li-ions on the electrode surface. The methodology and results in this work may boost the practical applicability of Li anodes in Li metal batteries and other battery systems using metal anodes.
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| 48. |
- Yang, Yang, et al.
(författare)
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Research progress on optimized membranes for vanadium redox flow batteries
- 2024
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Ingår i: Inorganic Chemistry Frontiers. - 2052-1553. ; 11:14, s. 4049-4079
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Forskningsöversikt (refereegranskat)abstract
- Energy storage systems are considered one of the key components for the large-scale utilization of renewable energy, which usually has an intermittent nature for production. In this case, vanadium redox flow batteries (VRFBs) have emerged as one of the most promising electrochemical energy storage systems for large-scale application, attracting significant attention in recent years. To achieve a high efficiency in VRFBs, the polymer electrolyte membrane between the positive and negative electrodes is expected to effectively transfer protons for internal circuits, and also prevent cross-over of the catholyte and anolyte. However, the high cost of membrane materials is currently a crucial factor restricting the large-scale application of VRFBs. In this review, key aspects related to the polymer electrolyte membranes in VRFBs are summarized, including their functional requirements, characterization methods, transport mechanisms, and classification. According to its classification, the latest research progress on the polymer electrolyte membrane in VRFBs is discussed in each section. Finally, the research directions and development of next-generation membrane materials for VRFBs are proposed, aiming to present a future perspective of this component in full batteries and inspire the ongoing efforts for building high-efficiency VRFBs in the power grid.
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| 49. |
- Yuan, Zijie, et al.
(författare)
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Study of the Corrosion Behavior of Cathode Current Collector in LiFSI Electrolyte
- 2024
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Ingår i: ChemSusChem. - 1864-5631 .- 1864-564X. ; In Press
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Tidskriftsartikel (refereegranskat)abstract
- Cycling aging is the one of the main reasons affecting the lifetime of lithium-ion batteries and the contribution of aluminum current collector corrosion to the ageing is not fully recognized. In general, aluminum is corrosion resistant to electrolyte since a non-permeable surface film of alumina is naturally formed. However, corrosion of aluminum current collector can still occur under certain conditions such as lithium bis(fluorosulfonyl)imide (LiFSI)-based electrolyte or high voltage. Herein, we investigates the corrosion of aluminum current collector in the electrolyte of 1.2 M LiFSI in ethylene carbonate (EC) and ethyl methyl carbonate (EMC) mixed solvents. The electrochemical results shows that the corrosion current of aluminum is enhanced by cycling time and potential, which is correlated with the surface species and morphology. The formation of AlF3, which is induced by deep penetration of F− anions through surface passivation film, leads to internal volume change and the surface crack in the end. Our work will be inspiring for future development of high-energy-density and high-power-density lithium-ion batteries in which the LiFSI salt will be intensively used.
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| 50. |
- Zhang, Chaofan, et al.
(författare)
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In Situ Volume Change Studies of Lithium Metal Electrode under Different Pressure
- 2019
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Ingår i: Journal of the Electrochemical Society. - : The Electrochemical Society. - 1945-7111 .- 0013-4651. ; 166:15, s. A3675-A3678
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Tidskriftsartikel (refereegranskat)abstract
- Due to the high theoretical capacity density of 3680 mAh g(-1), lithium (Li) is considered as a promising anode for high-energy-density battery systems. However, its practical application is severely hampered by the invariable growth of Li dendrites and tremendous volume change during electrochemical plating-stripping process. Although real-time monitoring of the volume change is crucial for research and development of stable lithium anode, the studies are rare due to the lack of in-situ swelling equipment so far. Here, we report an in-situ volume change system to observe the thickness change of Li electrode at a resolution of micrometer during the electrochemical process. With a comprehensive design for this instrument, a continuously tunable pressure can be applied on the Li-Li symmetric cell to investigate the impact of pressure on the stability of Li electrode during cycling. We found that the higher pressure (similar to 850kPa) is beneficial for stabilizing Li electrode during plating/stripping process. Our results provide a perspective to investigate the electrochemical behavior of Li electrode. In addition, this instrument also shows great potential of in-situ volume change monitoring in other battery systems like silicon anode and solid-state batteries.
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