| 1. |
- Hu, Jutao, et al.
(författare)
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The origin of anomalous hydrogen occupation in high entropy alloys
- 2022
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 10:13, s. 7228-7237
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Tidskriftsartikel (refereegranskat)abstract
- Metal hydrogen storage materials have been the focus of intensive research in the field of hydrogen-based economy. An outstanding question is that the number of hydrogen atoms accommodated in metal hydrides is generally much below the number of interstices, which limits their hydrogen storage capacities. Unlike traditional FCC metal hydrides where hydrogen can only occupy tetrahedral interstices, this study demonstrates that hydrogen can also occupy octahedral interstices in FCC high entropy alloy (HEA) hydrides, which leads to the violation of the Switendick criterion. For Ti25V25Nb25Ta25 and Ti25V25Nb25Zr25 HEAs, nearly 20% and 17.5% of octahedral interstices can be occupied by hydrogen, respectively. The anomalous hydrogen occupation mainly originates from the intrinsic electron delocalization between hydrogen atoms in HEA hydrides, which presents a sharp contrast to traditional metal hydrides. Such electron delocalization decreases repulsive interactions between hydrogens and promotes the electron localization at octahedral interstices. Additionally, this study reveals that hydrogen occupation at octahedral interstices enhances the structural disordering and decreases the thermal stability of HEA hydrides, which will be beneficial to reduce the dehydrogenation temperature. The presented results may provide a new strategy for the design of high-density storage materials.
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| 2. |
- Li, Xiane, et al.
(författare)
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Mapping the energy level alignment at donor/acceptor interfaces in non-fullerene organic solar cells
- 2022
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Ingår i: Nature Communications. - : Nature Portfolio. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- Energy level alignment (ELA) at donor-acceptor heterojunctions is of vital importance yet largely undetermined in organic solar cells. Here, authors determine the heterojunction ELA with (mono) layer-by-layer precision to understand the co-existence of efficient charge. Energy level alignment (ELA) at donor (D) -acceptor (A) heterojunctions is essential for understanding the charge generation and recombination process in organic photovoltaic devices. However, the ELA at the D-A interfaces is largely underdetermined, resulting in debates on the fundamental operating mechanisms of high-efficiency non-fullerene organic solar cells. Here, we systematically investigate ELA and its depth-dependent variation of a range of donor/non-fullerene-acceptor interfaces by fabricating and characterizing D-A quasi bilayers and planar bilayers. In contrast to previous assumptions, we observe significant vacuum level (VL) shifts existing at the D-A interfaces, which are demonstrated to be abrupt, extending over only 1-2 layers at the heterojunctions, and are attributed to interface dipoles induced by D-A electrostatic potential differences. The VL shifts result in reduced interfacial energetic offsets and increased charge transfer (CT) state energies which reconcile the conflicting observations of large energy level offsets inferred from neat films and large CT energies of donor - non-fullerene-acceptor systems.
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| 3. |
- Jiang, Kui, et al.
(författare)
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Suppressed recombination loss in organic photovoltaics adopting a planar-mixed heterojunction architecture
- 2022
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Ingår i: Nature Energy. - : NATURE PORTFOLIO. - 2058-7546. ; 7:11, s. 1076-1086
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Tidskriftsartikel (refereegranskat)abstract
- At present, high-performance organic photovoltaics mostly adopt a bulk-heterojunction architecture, in which exciton dissociation is facilitated by charge-transfer states formed at numerous donor-acceptor (D-A) heterojunctions. However, the spin character of charge-transfer states originated from recombination of photocarriers allows relaxation to the lowest-energy triplet exciton (T-1) at these heterojunctions, causing photocurrent loss. Here we find that this loss pathway can be alleviated in sequentially processed planar-mixed heterojunction (PMHJ) devices, employing donor and acceptor with intrinsically weaker exciton binding strengths. The reduced D-A intermixing in PMHJ alleviates non-geminate recombination at D-A contacts, limiting the chance of relaxation, thus suppressing T-1 formation without sacrificing exciton dissociation efficiency. This resulted in devices with high power conversion efficiencies of >19%. We elucidate the working mechanisms for PMHJs and discuss the implications for material design, device engineering and photophysics, thus providing a comprehensive grounding for future organic photovoltaics to reach their full promise. Organic solar cells with a bulk-heterojunction architecture suffer from photocurrent loss driven by triplet states. Now, Jiang et al. show that sequentially deposited donor-acceptor planar-mixed heterojunctions suppress triplet formation, enabling efficiencies over 19%.
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| 4. |
- Ma, Ruijie, et al.
(författare)
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All-polymer solar cells with over 16% efficiency and enhanced stability enabled by compatible solvent and polymer additives
- 2022
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Ingår i: Aggregate. - : Wiley. - 2692-4560 .- 2766-8541. ; 3:3
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Tidskriftsartikel (refereegranskat)abstract
- Considering the robust and stable nature of the active layers, advancing the power conversion efficiency (PCE) has long been the priority for all-polymer solar cells (all-PSCs). Despite the recent surge of PCE, the photovoltaic parameters of the state-of-the-art all-PSC still lag those of the polymer:small molecule-based devices. To compete with the counterparts, judicious modulation of the morphology and thus the device electrical properties are needed. It is difficult to improve all the parameters concurrently for the all-PSCs with advanced efficiency, and one increase is typically accompanied by the drop of the other(s). In this work, with the aids of the solvent additive (1-chloronaphthalene) and the n-type polymer additive (N2200), we can fine-tune the morphology of the active layer and demonstrate a 16.04% efficient all-PSC based on the PM6:PY-IT active layer. The grazing incidence wide-angle X-ray scattering measurements show that the shape of the crystallites can be altered, and the reshaped crystallites lead to enhanced and more balanced charge transport, reduced recombination, and suppressed energy loss, which lead to concurrently improved and device efficiency and stability.
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| 5. |
- Majed, Ahmad, et al.
(författare)
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Transition Metal Carbo-Chalcogenide "TMCC": A New Family of 2D Materials
- 2022
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Ingår i: Advanced Materials. - Weinheim, Germany : Wiley-VCH Verlagsgesellschaft. - 0935-9648 .- 1521-4095. ; 34:26
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Tidskriftsartikel (refereegranskat)abstract
- A new family of 2D transition metal carbo-chalcogenides (TMCCs) is reported, which can be considered a combination of two well-known families, TM carbides (MXenes) and TM dichalcogenides (TMDCs), at the atomic level. Single sheets are successfully obtained from multilayered Nb2S2C and Ta2S2C using electrochemical lithiation followed by sonication in water. The parent multilayered TMCCs are synthesized using a simple, scalable solid-state synthesis followed by a topochemical reaction. A superconductivity transition is observed at 7.55 K for Nb2S2C. The delaminated Nb2S2C outperforms both multilayered Nb2S2C and delaminated NbS2 as an electrode material for Li-ion batteries. Ab initio calculations predict the elastic constant of TMCC to be over 50% higher than that of TMDC.
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| 6. |
- Qi, Zhenyu, et al.
(författare)
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Blueshifting the Absorption of a Small -Molecule Donor and Using it as the Third Component to Achieve High-Efficiency Ternary Organic Solar Cells
- 2022
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Ingår i: Solar RRL. - : WILEY-V C H VERLAG GMBH. - 2367-198X. ; 6:9
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Tidskriftsartikel (refereegranskat)abstract
- Adding a small-molecule donor (SMD) to state-of-the-art nonfullerene organic solar cells (OSCs) is demonstrated as a useful strategy to construct ternary organic solar cells, as SMDs typically have high crystallinity and can tune charge transport properties of OSCs. However, the absorption of most SMDs overlaps with typical donor polymers (e.g., PM6), which is against the general guidelines of adopting materials with complementary absorption in ternary OSCs. Herein, the absorption of state-of-art SMDs (BTR-CI) by linking the beta position of the outer thiophene to the alpha position of the inner thiophene unit is intentionally blueshifted. The resulting molecule beta-S1 shows a maximum absorption peak at 505 nm in the film state, which exhibits wider bandgap and shows complementary absorption with the host system (PM6:Y6). The corresponding ternary OSCs with 20%wt beta-S1 show significantly enhanced efficiency from 16.2% to 17.1% due to the increased short-circuit current (J(sc)) and improved fill factor (FF). Herein, an effective strategy to design SMDs with both wider bandgaps and higher crystallinity for high-performance ternary OSCs is presented.
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| 7. |
- Wei, Zhongbao, et al.
(författare)
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Multi-stage state of health estimation of lithium-ion battery with high tolerance to heavily-partial charging
- 2022
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Ingår i: IEEE Transactions on Power Electronics. - 0885-8993 .- 1941-0107. ; 37:6, s. 7432-7442
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Tidskriftsartikel (refereegranskat)abstract
- State of health (SOH) is critical to the management of lithium-ion battery (LIB) due to its deep insight into the health diagnostic and protection. However, the absence of complete charging data, which is common in practice, risks impairing the charging-based SOH estimators. This paper proposes a multi-stage SOH estimation method with a broad scope of applications, including the unfavorable but practical scenarios of heavily-partial charging. In particular, different sets of health indicators (HIs), covering both the morphological IC features and the voltage entropy information, are extracted from the partial CC charging data with different initial charging voltage to characterize the aging status. Following this endeavor, artificial neural network (ANN)-based HI fusion is proposed to estimate the SOH of LIB precisely in real time. The proposed method is evaluated with long-term aging experiments performed on different types of LIBs. Results validate several superior merits of the proposed method, including high estimation accuracy, high tolerance to partial charging, strong robustness to cell inconsistency, and wide generality to different battery types.
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| 8. |
- Zhang, Jianwei, et al.
(författare)
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Electrochemical Palladium-Catalyzed Oxidative Carbonylation-Cyclization of Enallenols
- 2022
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 61:49
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we report an electrochemical oxidative palladium-catalyzed carbonylation-carbocyclization of enallenols to afford gamma-lactones and spirolactones, which proceeds with excellent chemoselectivity. Interestingly, electrocatalysis was found to have an accelerating effect on the rate of the tandem process, leading to a more efficient reaction than that under chemical redox conditions.
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| 9. |
- Zhang, Xin, et al.
(författare)
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High-Performance All-Small-Molecule Organic Solar Cells Enabled by Regio-Isomerization of Noncovalently Conformational Locks
- 2022
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Ingår i: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 32:19
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Tidskriftsartikel (refereegranskat)abstract
- The power conversion efficiencies (PCEs) of organic solar cells (OSCs) have surpassed 19% thanks to the innovation of polymer donors and molecular acceptors. However, the batch-to-batch variations in polymer materials are detrimental to the reproducibility of the device performance. In comparison, small-molecule donors (SMDs) possess some unique advantages, such as well-defined molecular weights, easy purification, and excellent batch-to-batch repeatability. Herein, a pair of regioisomeric SMDs (BT-O1 and BT-O2) has been synthesized with alkoxy groups as S center dot center dot center dot O noncovalently conformational locks (NoCLs) at the inner and outer position, respectively. Theoretical and experimental results reveal that the regioisomeric effect has a significant influence on the light-harvest ability, energy levels, molecular geometries, internal reorganization energy, and packing behaviors for the two SMDs. As a result, BT-O2-based binary device shows an impressive PCE of 13.99%, much higher than that of BT-O1 based one (4.07%), due to the better-aligned energy level, more balanced charge transport, less charge recombination, lower energy loss, and more favorable phase separation. Furthermore, the fullerene derivative PC71BM is introduced into BT-O2:H3 as the third component to achieve a notable PCE of 15.34% (certified 14.6%). Overall, this work reveals that NoCLs is a promising strategy to achieve high-performance SMDs for all-small-molecule OSCs.
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