Filling the Gap between Heteroatom Doping and Edge Enrichment of 2D Electrocatalysts for Enhanced Hydrogen Evolution

Wang, Wenbin1,2; Song, Yun3,4; Ke, Chengxuan2,5; Li, Yang3,4; Liu, Yong3,4; Ma, Chen6; Wu, Zongxiao2; Qi, Junlei2; Bao, Kai2; Wang, Lingzhi2; Wu, Jingkun2; Jiang, Shan7; Zhao, Jiong7; Lee, Chun-Sing4,8,9; Chen, Ye6; Luo, Guangfu10; He, Qiyuan2; Ye, Ruquan1,3,4

2023

10.1021/acsnano.2c09423

ACS Nano   影响因子和分区

1936-0851

1936-086X

Composition modulation and edge enrichment are established protocols to steer the electronic structures and catalytic activities of twodimensional (2D) materials. It is believed that a heteroatom enhances the catalytic performance by activating the chemically inert basal plane of 2D crystals. However, the edge and basal plane have inherently different electronic states, and how the dopants affect the edge activity remains ambiguous. Here we provide mechanistic insights into this issue by monitoring the hydrogen evolution reaction (HER) performance of phosphorus-doped MoS2 (P-MoS2) nanosheets via on-chip electrocatalytic microdevices. Upon phosphorus doping, MoS2 nanosheet gets catalytically activated and, more importantly, shows higher HER activity in the edge than the basal plane. In situ transport measurement demonstrates that the improved HER performance of P-MoS2 is derived from intrinsic catalytic activity rather than charge transfer. Density functional theory calculations manifest that the edge sites of PMoS2 are energetically more favorable for HER. The finding guides the rational design of edge-dominant P-MoS2, reaching a minuscule onset potential of similar to 30 mV and Tafel slope of 48 mV/dec that are benchmarked against other activation methods. Our results disclose the hitherto overlooked edge activity of 2D materials induced by heteroatom doping that will provide perspectives for preparing next-generation 2D catalysts.

Active edge sites basal plane heteroatom doping on-chip electrochemistry hydrogen evolution reaction

SCI

英语

NI论文

通讯

National Natural Science Foundation of China[21905240] ; Guangdong Basic and Applied Basic Research Fund[2022A1515011333] ; Shenzhen Science and Technology Program["2021Szvup129","JCYJ20220818"] ; Hong Kong Research Grant Council["21300620","11307120","9229079","9610482","7005468"] ; City University of Hong Kong["21302821","11314322"] ; Guangdong Provincial Key Laboratory of Computational Science and Material Design[2019B030301001] ; Introduced Innovative R&D Team of Guangdong[2017ZT07C062] ; Shenzhen Science and Technology Innovation Committee[JCYJ20200109141412308]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000919117000001

AMER CHEMICAL SOC

Web of Science

1.City Univ Hong Kong, Shenzhen Res Inst, Shenzhen 518057, Guangdong, Peoples R China
2.City Univ Hong Kong, Dept Mat Sci & Engn, Kowloon, Hong Kong, Peoples R China
3.City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
4.City Univ Hong Kong, State Key Lab Marine Pollut, Hong Kong, Peoples R China
5.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
6.Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China
7.Hong Kong Polytech Univ, Dept Appl Phys, Hong Kong, Peoples R China
8.City Univ Hong Kong, Dept Chem, Hong Kong, Peoples R China
9.City Univ Hong Kong, Ctr Superdiamond & Adv Films COSDAF, Hong Kong, Peoples R China
10.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Guangdong, Peoples R China

Wang, Wenbin,Song, Yun,Ke, Chengxuan,et al. Filling the Gap between Heteroatom Doping and Edge Enrichment of 2D Electrocatalysts for Enhanced Hydrogen Evolution[J]. ACS Nano,2023,17(2).

Wang, Wenbin.,Song, Yun.,Ke, Chengxuan.,Li, Yang.,Liu, Yong.,...&Ye, Ruquan.(2023).Filling the Gap between Heteroatom Doping and Edge Enrichment of 2D Electrocatalysts for Enhanced Hydrogen Evolution.ACS Nano,17(2).

Wang, Wenbin,et al."Filling the Gap between Heteroatom Doping and Edge Enrichment of 2D Electrocatalysts for Enhanced Hydrogen Evolution".ACS Nano 17.2(2023).