| 1. |
- Chen, Zhiwen, et al.
(författare)
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Interface engineering of NiS@MoS2 core-shell microspheres as an efficient catalyst for hydrogen evolution reaction in both acidic and alkaline medium
- 2021
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Ingår i: Journal of Alloys and Compounds. - : ELSEVIER SCIENCE SA. - 0925-8388 .- 1873-4669. ; 853
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical splitting of water is one of the most reliable and effective ways for the sustainable production of pure hydrogen on a large scale, while the core of this technology lies in the development of highly active non-noble-metal-based electrocatalysts to lower the large dynamic overpotentials of electrode materials. Here, an interface engineering strategy is demonstrated to construct an efficient and stable catalyst based on NiS@MoS2 core-shell hierarchical microspheres for the hydrogen evolution reactions (HER). The ultrathin MoS2 nanosheets in-situ grow on the surface of NiS hierarchical micro-sized spheres constructed by porous nanoplates, endowing the composites with rich interfaces, well-exposed electroactive edges, high structural porosity and fast transport channels. These advantages are favorable for the improvement of catalytic sites and the transport of catalysis-relevant species. More importantly, the intimate contact between MoS2 nanosheets and NiS nanoplates synergistically favors the chemical sorption of hydrogen intermediates, thereby reducing the reaction barrier and accelerating the HER catalytic process. As a result, the optimized NiS@MoS2 catalyst manifests impressive HER activity and durability, with a low overpotential of 208 mV in 0.5 M H2SO4 and 146 mV in 1.0 M KOH at 10 mA cm(-2), respectively. This work not only provides an effective way to construct core-shell hierarchical microspheres but also a multiscale strategy to regulate the electronic structure of heterostructured materials for energy-related applications. (C) 2020 Elsevier B.V. All rights reserved.
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| 2. |
- Chen, Zhiwen, et al.
(författare)
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Well-defined CoSe2@MoSe2 hollow heterostructured nanocubes with enhanced dissociation kinetics for overall water splitting
- 2020
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Ingår i: Nanoscale. - : ROYAL SOC CHEMISTRY. - 2040-3364 .- 2040-3372. ; 12:1, s. 326-335
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Tidskriftsartikel (refereegranskat)abstract
- Hollow heterostructures have tremendous advantages in electrochemical energy storage and conversion areas due to their unique structure and composition characteristics. Here, we report the controlled synthesis of hollow CoSe2 nanocubes decorated with ultrathin MoSe2 nanosheets (CoSe2@MoSe2) as an efficient and robust bifunctional electrocatalyst for overall water splitting in a wide pH range. It is found that integrating ultrathin MoS2 nanosheets with hollow CoSe2 nanocubes can provide abundant active sites, promote electron/mass transfer and bubble release and facilitate the migration of charge carriers. Additionally, the surface electron coupling in the heterostructures enables it to serve as a source of sites for H+ and/or OH- adsorption, thus reducing the activation barrier for water molecules adsorption and dissociation. As a result, the title compound, CoSe2@MoSe2 hollow heterostructures, exhibits an overpotential of 183 mV and 309 mV at a current density of 10 mA cm(-2) toward hydrogen evolution reactions and oxygen evolution reactions in 1.0 M KOH, respectively. When applied as both cathode and anode for overall water splitting, a low battery voltage of 1.524 V is achieved along with excellent stability for at least 12 h. This work provides a new idea for the design and synthesis of high-performance catalysts for electrochemical energy storage and conversion.
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| 3. |
- Deng, Min, et al.
(författare)
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Genome-wide association analyses in Han Chinese identify two new susceptibility loci for amyotrophic lateral sclerosis
- 2013
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Ingår i: Nature Genetics. - : Nature Publishing Group. - 1061-4036 .- 1546-1718. ; 45:6, s. 697-
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Tidskriftsartikel (refereegranskat)abstract
- To identify susceptibility genes for amyotrophic lateral sclerosis (ALS), we conducted a genome-wide association study (GWAS) in 506 individuals with sporadic ALS and 1,859 controls of Han Chinese ancestry. Ninety top SNPs suggested by the current GWAS and 6 SNPs identified by previous GWAS were analyzed in an independent cohort of 706 individuals with ALS and 1,777 controls of Han Chinese ancestry. We discovered two new susceptibility loci for ALS at 1q32 (CAMK1G, rs6703183, P-combined = 2.92 x 10(-8), odds ratio (OR) = 1.31) and 22p11 (CABIN1 and SUSD2, rs8141797, P-combined = 2.35 x 10(-9), OR = 1.52). These two loci explain 12.48% of the overall variance in disease risk in the Han Chinese population. We found no association evidence for the previously reported loci in the Han Chinese population, suggesting genetic heterogeneity of disease susceptibility for ALS between ancestry groups. Our study identifies two new susceptibility loci and suggests new pathogenic mechanisms of ALS.
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| 4. |
- Huang, Shoushuang, et al.
(författare)
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An advanced electrocatalyst for efficient synthesis of ammonia based on chemically coupled NiS@MoS2 heterostructured nanospheres
- 2021
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Ingår i: Sustainable Energy & Fuels. - : Royal Society of Chemistry. - 2398-4902. ; 5:10, s. 2640-2648
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Tidskriftsartikel (refereegranskat)abstract
- The electrochemical reduction of nitrogen, as a sustainable alternative to the known Haber-Bosch process, possesses promising application prospects in the development of renewable energy storage systems. However, the yield of NH3 and Faraday efficiency are usually very low owing to the loss of active electrocatalysts and competitive hydrogen evolution reactions. Herein, uniform NiS@MoS2 core-shell microspheres are controllably prepared as a potential catalyst for an ambient electrocatalytic N-2 reduction reaction. The NiS@MoS2 microspheres possess highly active intrinsic, sufficient accessible active sites, high structural porosity, and convenient transport channels, consequently boosting the transmission of electrons and mass. Additionally, the interfacial interaction between NiS and MoS2 facilitates electron transfer, which further improves the catalytic activity by optimizing the free energies of reaction intermediates. As a result, the titled NiS@MoS2 shows excellent electrochemical activity and selectivity, capable of achieving a relatively high NH3 yield of 9.66 mu g h(-1) mg(cat)(-1) at -0.3 V (vs. the reversible hydrogen electrode, RHE) and a high FE of 14.8% at -0.1 V vs. RHE in 0.1 M Na2SO4. The work demonstrated here may open a new avenue for the rational design and synthesis of catalysts for the electrochemical synthesis of ammonia.
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| 5. |
- Huang, Shoushuang, et al.
(författare)
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Synergistically modulating electronic structure of NiS2 hierarchical architectures by phosphorus doping and sulfur-vacancies defect engineering enables efficient electrocatalytic water splitting
- 2021
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Ingår i: Chemical Engineering Journal. - : ELSEVIER SCIENCE SA. - 1385-8947 .- 1873-3212. ; 420
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Tidskriftsartikel (refereegranskat)abstract
- The synergistic achievement of heteroatom doping, defect engineering and appropriate structural design is efficient to adjust and boost the catalytic performance of catalysts yet challenging. Herein, phosphorus (P)-doped NiS2 hierarchical architectures with sulfur vacancies are synthesized via a Prussian-blue-analogue-sacrificed strategy followed by a phosphidation process. By modulation of P doping and sulfur vacancies, the optimal catalyst manifests outstanding electrocatalytic activities, affording low overpotentials of 73 mV at 10 mA cm-2 for hydrogen evolution reaction (HER), and 255 mV at 20 mA cm-2 for oxygen evolution reaction (OER), respectively. Density functional theory calculations certify that the P dopant not only serves as the new active sites, but also activates the electrochemical activity of neighboring Ni and S sites. Moreover, the synergistic effect of P-doping and sulfur vacancies further improve electrochemical activities of HER and OER by optimizing the adsorption free energy of hydrogen (Delta GH*) and oxygen-containing intermediates (OH*, O* and OOH*), respectively. This finding provides a directive strategy to achieve efficient non-noble metal catalysts for energy conversion and storage.
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| 6. |
- Le, Thanh-Tung, et al.
(författare)
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Phosphorus-doped Fe7S8@C nanowires for efficient electrochemical hydrogen and oxygen evolutions: Controlled synthesis and electronic modulation on active sites
- 2021
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Ingår i: Journal of Materials Science & Technology. - : JOURNAL MATER SCI TECHNOL. - 1005-0302. ; 74, s. 168-175
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Tidskriftsartikel (refereegranskat)abstract
- Developing low-cost, efficient, and stable non-precious-metal electrocatalysts with controlled crystal structure, morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions. Herein, a series of phosphorus-doped Fe7S8 nanowires integrated within carbon (P-Fe7S8@C) are rationally synthesized via a one-step phosphorization of one-dimensional (1D) Fe-based organic-inorganic nanowires. The as-obtained P-Fe7S8@C catalysts with modified electronic configurations present typical porous structure, providing plentiful active sites for rapid reaction kinetics. Density functional calculations demonstrate that the doping Fe7S8 with P can effectively enhance the electron density of Fe7S8 around the Fermi level and weaken the Fe-H bonding, leading to the decrease of adsorption free energy barrier on active sites. As a result, the optimal catalyst of P-Fe7S8-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction (HER) to reach the current density of 10 mA/cm(2), and a significantly low overpotential of 210 mV for oxygen evolution reaction (OER) at 20 mA/cm(2) in alkaline media. The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation. (C) 2021 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
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| 7. |
- Ma, Chunyan, et al.
(författare)
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CO2 capture using ionic liquid-based hybrid solvents from experiment to process evaluation
- 2021
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Ingår i: Applied Energy. - : Elsevier. - 0306-2619 .- 1872-9118. ; 304
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Tidskriftsartikel (refereegranskat)abstract
- The CO2 absorption capacity in three hybrid solvents based on butyl-3-methylimidazolium acetate ([Bmim][OAc]) and three different cosolvents (Dimethyl ethers of polyethylene glycol (DEPG250), propylene carbonate, and water) was investigated and compared, and [Bmim][OAc]-DEPG250 shows the highest CO2 absorption capacity. The effects of the mass ratio of [Bmim][OAc]-DEPG250 and temperature on their CO2 absorption capacity, density, and viscosity were further investigated. In addition, the absorption capacities of N2 and CO2 in [Bmim][OAc]-DEPG250 with the simulated flue gas as a feed gas were studied and compared with that using the pure gas as a feed gas. Thermodynamic models were used to represent the experimental data, and then process simulation and evaluation were carried out. The results show that the addition of DEPG250 dramatically decreases the viscosity, while the absorption capacity of hybrid solvents is still comparable with pure [Bmim][OAc]. The type of gas stream, that is, pure gas or gas mixture, has a negligible effect on the N2 and CO2 absorption capacity. The simulation results show that [Bmim][OAc]-DEPG250 only utilizes less than 50% of the heating duty of aqueous amine solution because of the low-pressure desorption and preheating with waste heat in this hybrid solvent-based process. The CO2 capture cost of using this [Bmim][OAc]-DEPG250 reduces by 11% compared with that of using aqueous amine solution due to the significant decrease (by 52%) in utility cost.
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| 8. |
- Mittler, Eva, et al.
(författare)
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Structural and mechanistic basis of neutralization by a pan-hantavirus protective antibody
- 2023
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Ingår i: Science Translational Medicine. - : American Association for the Advancement of Science (AAAS). - 1946-6234 .- 1946-6242. ; 15:700
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Tidskriftsartikel (refereegranskat)abstract
- Emerging rodent-borne hantaviruses cause severe diseases in humans with no approved vaccines or therapeutics. We recently isolated a monoclonal broadly neutralizing antibody (nAb) from a Puumala virus-experienced human donor. Here, we report its structure bound to its target, the Gn/Gc glycoprotein heterodimer comprising the viral fusion complex. The structure explains the broad activity of the nAb: It recognizes conserved Gc fusion loop sequences and the main chain of variable Gn sequences, thereby straddling the Gn/Gc heterodimer and locking it in its prefusion conformation. We show that the nAb's accelerated dissociation from the divergent Andes virus Gn/Gc at endosomal acidic pH limits its potency against this highly lethal virus and correct this liability by engineering an optimized variant that sets a benchmark as a candidate pan-hantavirus therapeutic.
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| 9. |
- Wang, Nan, et al.
(författare)
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CO2 separation from biogas with ionic liquid-based hybrid solvents: From properties to process
- 2022
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Ingår i: Separation and Purification Technology. - : Elsevier. - 1383-5866 .- 1873-3794. ; 298
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Tidskriftsartikel (refereegranskat)abstract
- In this work, ionic liquids (ILs)-based hybrid solvents, consisting of 1-butyl-3-methylimidazolium acetate (BMAC)-propylene carbonate (PC), were developed for CO2 separation from biogas. The impacts of IL mass fraction and temperature on the absorption capacity, viscosity, and density were studied. Feed gases, including pure CO2, pure CH4, and synthetic biogas, were tested, and the results were evaluated and compared. Thermodynamic modeling was used to represent the newly measured results together with literature data, and a systematic process simulation and evaluation were conducted. The measurements show an enhanced CO2 solubility with an increased BMAC mass fraction and decreased temperature. An increased viscosity was observed with increasing BMAC mass fraction and decreasing temperature. In addition, the type of feed gas holds a neglectable effect on CO2 and CH4 absorption capacities. To find an optimal mass fraction of BMAC-PC and quantify the performance, in the process simulation and evaluation, two types of regeneration blocks, i.e., air-blow regeneration and thermal regeneration, were involved. It shows that the process with thermal regeneration block requires less energy and lower capture cost than the process with the air-blow regeneration, which indicates a superior affinity to thermal regeneration when BMAC is presented in the solvent system. Also, the decrease in PC content firstly decreases and then increases the energy demand, and the minimum energy demand of 23.4 kW can be found with wIL=0.3, which reduces by 33.5% compared to pure PC. Similarly, the minimum capture cost of 68 $/ton-CO2 can be found with wIL=0.3, representing a 21% reduction from the case with pure PC. The further analysis concludes a major reduction in the utility cost by 48%.
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