Universal construction of sulfur doped molybdenum-based nanosheets for enhanced hydrogen evolution in a wide pH range
Universal construction of sulfur doped molybdenum-based nanosheets for enhanced hydrogen evolution in a wide pH range
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DOI：
10.1016/j.apcatb.2022.122131
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Ming-hao Hu;Baocang Liu;Heng Chen;Xuang-Long Xu;P. Jing;Xiaolei Guo;Rui Yang;Xiaoyang Wang
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文献类型：
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作者：
Ming-hao Hu;Baocang Liu;Heng Chen;Xuang-Long Xu;P. Jing;Xiaolei Guo;Rui Yang;Xiaoyang Wang
合理设计和制备具有丰富暴露活性中心和优化电子结构的催化剂是提高电催化性能的关键。在本研究中，通过对MoS2纳米片进行原位拓扑变换，在碳布上普遍构建了有序的多孔含硫钼基化合物纳米片(S-MoXn/CC，S-MoXn=S-MoP，S-Mo2C，S-MON和S-MoO_3)，作为pH普适析氢反应(HER)的自支撑电极。各种结构表征表明，具有丰富的纳米孔和边缘的S-MoXn纳米片具有丰富的暴露的活性中心，高的传质效率和良好的导电性。结果表明，在酸性、碱性和中性电解液中，S-MoXn/CC电极，特别是S-MOP/CC电极在10 mA/cm−时的过电位分别为75、75和127mV，表现出优异的性能，优于MoXn/CC电极。理论计算表明，S掺杂和MoXn之间的协同作用可以有效地改变S-MoXn的电子结构，从而提高她的性能。
Rational designing and fabricating catalysts with abundant exposed active sites and optimized electronic structure is of essential to boost electrocatalytic performance. In this study, well-organized porous nanosheets of sulfur-doped molybdenum-based compounds on carbon cloth (S-MoXn/CC, S-MoXn= S-MoP, S-Mo2C, S-MoN, and S-MoO3) are universally constructed via in situ topological transformation from the MoS2nanosheets as self-supported electrodes for pH-universal hydrogen evolution reaction (HER). Various structural characterizations show that the S-MoXnnanosheets with abundant nanopores and edges endowing them with plentiful exposed active sites, high mass transfer efficiency, and good conductivity. As a result, these S-MoXn/CC electrodes, especially S-MoP/CC exhibits superior HER performance with low overpotentials of 75, 75, and 127 mV at 10 mA cm−1in acidic, alkaline, and neutral electrolytes, superior to the MoXn/CC counterparts. Theoretical calculations reveal that the synergy between S dopant and MoXncan effectively alter the electronic structure of S-MoXn, thus enhancing the HER performance.