Coral-shaped Mn-CuS with hierarchical pores and crystalline defects for high-efficiency H2O2 production via electrocatalytic two-electron reduction
Coral-shaped Mn-CuS with hierarchical pores and crystalline defects for high-efficiency H2O2 production via electrocatalytic two-electron reduction
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DOI:
10.1016/j.apcatb.2023.122721
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发表时间:
2023
期刊:
影响因子:
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通讯作者:
Ao Zhang;Zhongqing Jiang;Shaoda Zhang;Penghua Lan;Naihua Miao;Weiheng Chen;Ning Huang;Xiaoning Tian;Yangjie Liu;Zhongyu Cai
中科院分区:
文献类型:
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作者:
Ao Zhang;Zhongqing Jiang;Shaoda Zhang;Penghua Lan;Naihua Miao;Weiheng Chen;Ning Huang;Xiaoning Tian;Yangjie Liu;Zhongyu Cai
We report the development of non-noble transition metal sulfide catalysts Mn-CuS-x for high-efficiency and selective H2O2production. In this study, we synthesized Mn-CuS-x with coral-shaped hierarchical porous structure through one-pot hydrothermal reaction. The Mn-CuS-x possesses large specific surface area with plenty of crystalline defects via heteroatom doping of Mn. The Mn-CuS-x kinetically favored 2e−pathway over 4e−pathway, resulting in high selectivity (>92%) to H2O2production and high H2O2concentration (∼24.5 mM at 0.6 V vs. RHE) within 3 h for the optimized Mn-CuS-2 catalysts (synthesized with a molar ratio of 1:3:8 (MnCl2·4 H2O: CuCl2·2 H2O: C2H5NS)). The Mn-CuS-2 showed excellent stability, indicating that the Mn-CuS electrocatalysts can simultaneously achieve both high stability and enhanced H2O2production. Our first-principles calculations further confirmed that the heteroatom Mn doping to CuS thermodynamically makes the 2e–-ORR pathway more favorable. This study provides a green, low-cost, and efficient route to produce H2O2, which is very promising for generating chemicals and liquid fuels.