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34. Progress on the Design of Electrocatalysts for Large‐Current Hydrogen Production by Tuning Thermodynamic and Kinetic Factors.

Author

Li, Ye, Feng, Ao, Dai, Linxiu, Xi, Baojuan, An, Xuguang, Xiong, Shenglin, and An, Changhua

Subjects
HYDROGEN production, ELECTROCATALYSTS, GREEN fuels, CARBON offsetting, HYDROGEN evolution reactions, CHARGE transfer, MASS transfer
Abstract

Electrochemical water splitting to produce green hydrogen offers a promising technology for renewable energy conversion and storage, as well as realizing carbon neutrality. The efficiency, stability, and cost of electrocatalysts toward hydrogen evolution reaction (HER) and electrocatalytic overall water splitting (EOWS) at large current densities are essential for practical application. In this review, the key factors that determine the catalytic performance of electrocatalysts at large current densities are summarized from the angel of thermodynamic and kinetic correlation. The corresponding design strategies are presented. The electronic structure and density of active sites that affect the adsorption/desorption of intermediates are considered as the thermodynamic aspects, while charge transfer and mass transport capabilities closely associated with electrode resistance and intermediate diffusion are assigned as kinetic effects. Recent development of bifunctional and integrated electrocatalysts toward EOWS is also discussed in detail. Finally, the perspective and direction on the electrocatalytic water splitting under large current density are proposed. This comprehensive overview will offer profound insights and guidance for the continued advancement of this field. [ABSTRACT FROM AUTHOR]

Published
2024
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43. Molecular‐Level Design of High Flash Point Solvents Enables High‐Safety and Dual‐Function Chemical Presodiation of Hard Carbon and Alloy Anodes for High‐Performance Sodium‐Ion Batteries.

Author

Man, Quanyan, Wei, Chuanliang, Tian, Kangdong, Shen, Hengtao, Zhang, Xinlu, Bai, Xuexiu, Xi, Baojuan, Xiong, Shenglin, and Feng, Jinkui

Subjects
SODIUM ions, KINETIC energy, REDUCTION potential, ENERGY density, SOLVENTS, LITHIUM cells, ELECTRIC batteries, ANODES
Abstract

Hard carbon (HC) is subjected to low initial Coulombic efficiency (ICE) and unsteady solid electrolyte interphase (SEI), which limits the energy density and cycling performance. Meanwhile, studies related to emerging chemical presodiation have specifically focused on proper redox potential and overlooked its safety hazard. To address these drawbacks of HC and chemical presodiation, a series of high‐safety chemical presodiation solutions based on tetraethylene glycol dimethyl ether (TEGDME) are proposed for uniform and fast presodiation of HC and Bi anodes. Among them, Na‐4‐methylbiphenyl in TEGDME solution exhibits the lowest redox potential (0.146 V vs Na+/Na), which achieves the inhibition of initial irreversible sodium uptake. Meantime, the potential‐driven decomposition of fluoroethylene carbonate endows presodiated HC (pNa‐HC) a fast‐ion conducting and robust F‐rich SEI. Accordingly, pNa‐HC delivers an ideal ICE of 99.1% compared to HC (65.28%). Meanwhile, pNa‐HC exhibits significantly enhanced rate performance and cycling life (193.39 mAh g−1 after 2300 cycles at 1000 mA g−1) benefiting from reduced kinetic energy barriers. When pNa‐HC pairs with Na3V2(PO4)3 cathode, the full cell demonstrates a desirable ICE of 91.25%. This work provides a novel and universal solvent design strategy to realize high‐safety chemical pre‐metallation. [ABSTRACT FROM AUTHOR]

Published
2024
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47. Synchronous Regulation of D–Band Centers in Zn Substrates and Weakening Pauli Repulsion of Zn Ions Using the Ascorbic Acid Additive for Reversible Zinc Anodes.

Author

Zhang, Zhengchunyu, Wang, Peng, Wei, Chuanliang, Feng, Jinkui, Xiong, Shenglin, and Xi, Baojuan

Subjects
VITAMIN C, HYDROGEN evolution reactions, AQUEOUS electrolytes, ANODES, IONIC structure
Abstract

The advanced aqueous zinc–ion batteries (AZIBs) are still challenging due to the harmful reactions including hydrogen evolution and corrosion. Here, a natural small molecule acid vitamin C (Vc) as an aqueous electrolyte additive has been selectively identified. The small molecule Vc can adjust the d band center of Zn substrate which fixes the active H+ so that the hydrogen evolution reaction (HER) is restrained. Simultaneously, it could also fine–tune the solvation structure of Zn ions due to the enhanced electrostatics and reduced Pauli repulsion verified by energy decomposition analysis (EDA). Hence, the cell retains an ultra–long cycle performance of over 1300 cycles and a superior Coulombic efficiency (CE) of 99.5 %. The prepared full cells display increased rate capability, cycle lifetime, and self–discharge suppression. Our results shed light on the mechanistic principle of electrolyte additives on the performance improvement of ZIBs, which is anticipated to render a new round of studies. [ABSTRACT FROM AUTHOR]

Published
2024
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48. Heterostructure of 2D MoSe2 nanosheets vertically grown on bowl-like carbon for high-performance sodium storage.

Author

Shi, Nianxiang, Liu, Guangzeng, Xi, Baojuan, An, Xuguang, Sun, Changhui, and Xiong, Shenglin

Subjects
NANOSTRUCTURED materials, SODIUM ions, SODIUM, TRANSITION metal oxides, TRANSITION metals, CHEMICAL kinetics
Abstract

Transition metal dichalcogenides are attractive anode materials for sodium ion batteries (SIBs) due to their high theoretical capacity and large interlayer spacing. However, its practical application is hampered by the sluggish kinetics of Na+ insertion and structure collapse caused by Na+ insertion/deinsertion. Herein, the heterostructures of MoSe2 nanosheets vertically growing on bowl-like carbon (MoSe2@C) are designed and prepared by a template method coupled with selenization treatment to boost storage sodium performance. The hollow and collapse could provide enough storage space for Na+ and alleviate the volume expansion during the charge/discharge processes. MoSe2 nanosheets vertically grown on carbon could expose more active sites for adsorbing Na+ to enhance the utilization rate of electrode materials. Moreover, building heterostructures by combining different phase components could facilitate Na+ diffusion and advance reaction kinetics. Benefiting from these merits, the bowllike MoSe2@C shows outstanding reversible capacity (356.8 mAh·g−1 after 1500 cycles at 1 A·g−1) and remarkable rate performance (249.9 mAh·g−1 10 A·g−1). [ABSTRACT FROM AUTHOR]

Published
2024
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