Enhancing the Performance of Bi_2S_3 in Electrocatalytic and Supercapacitor Applications by Controlling Lattice Strain

Hao Zhang; Jiefeng Diao; Mengzheng OuyangHossein YadegariMingxuan MaoJiaao WangGraeme HenkelmanFang XieDavid Jason Riley

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Enhancing the Performance of Bi_2S_3 in Electrocatalytic and Supercapacitor Applications by Controlling Lattice Strain

机译：Enhancing the Performance of Bi_2S_3 in Electrocatalytic and Supercapacitor Applications by Controlling Lattice Strain

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Lattice-strained Bi_2S_3 with 3D hierarchical structures are prepared through a top-down route by a topotactic transformation. High-resolution transmission electron microscopy and X-ray diffraction (XRD) confirm the lattice spacing is expanded by prolonged sulfuration. Performance studies demonstrate that Bi_2S_3 with the largest lattice expansion (Bi_2S_3-9.7%, where 9.7% represents the lattice expansion) exhibits a greater electrocatalytic hydrogen evolution reaction (HER) activity compared to Bi_2S_3 and Bi_2S_3-3.2%. Density functional theory calculations reveal the expansion of the lattice spacing reduces the bandwidth and upshifts the band center of the Bi 3d orbits, facilitating electron exchange with the S 2p orbits. The resultant intrinsic electronic configuration exhibits favorable H* adsorption kinetics and a reduced energy barrier for water dissociation in hydrogen evolution. Operando Raman and postmortem characterizations using XRD and X-ray photoelectron spectroscopy reveal the generation of pseudo-amorphous Bi at the edge of Bi_2S_3 nanorods of the sample with lattice strain during HER, yielding Bi_2S_3-9.7%-A. It is worth noting when Bi_2S_3-9.7%-A is assembled as a positive electrode in an asymmetric supercapacitor, its performance is greatly superior to that of the same device formed using pristine Bi_2S_3-9.7%. The as-prepared Bi_2S_3-9.7%-A//activated carbon asymmetric supercapacitor achieves a high specific capacitance of 307.4 F g~(?1) at 1 A g~(?1), exhibiting high retention of 84.1% after 10 000 cycles.

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《Advanced functional materials》 |2022年第48期|2205974.1-2205974.12|共12页
作者
Hao Zhang; Jiefeng Diao; Mengzheng OuyangHossein YadegariMingxuan MaoJiaao WangGraeme HenkelmanFang XieDavid Jason Riley;
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Department of Materials and London Center for Nanotechnology Imperial College London London SW7 2AZ, UK;

Department of Chemistry and the Oden Institute for Computational Engineering and Sciences The University of Texas at Austin Austin, TX 78712, USA;

Department of Earth Science and Engineering Imperial College London London SW7 2AZ, UKDepartment of Electrical and Electronic Engineering Imperial College London London SW7 2AZ, UK;

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asymmetric supercapacitors; bismuth sulfide; lattice strain; pH universal; seawater hydrogen evolution reaction;

Enhancing the Performance of Bi_2S_3 in Electrocatalytic and Supercapacitor Applications by Controlling Lattice Strain

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