Auto-optimizing Hydrogen Evolution Catalytic Activity of ReS2 through Intrinsic Charge Engineering

doi:10.1021/acsnano.8b00693

	Auto-optimizing Hydrogen Evolution Catalytic Activity of ReS2 through Intrinsic Charge Engineering
	Zhou, Yao ; Song, Erhong ; Zhou, Jiadong 1; Lin, Junhao 2; Ma, Ruguang ; Wang, Youwei ; Qiu, Wujie ; Shen, Ruxiang ; Suenaga, Kazutomo 2; Liu, Qian 3
刊名	ACS NANO
	2018
卷号	12 期号:5 页码:4486
关键词	monolayer transition metal dichalcogenides metal-metal bonds theoretical calculation hydrogen evolution reaction
ISSN号	1936-0851
DOI	10.1021/acsnano.8b00693
英文摘要	Optimizing active electronic states responding to catalysis is of paramount importance for developing high-activity catalysts because thermodynamics itself may not favor forming an optimal electronic state. Setting the monolayer transition metal dichalcogenide (TMD) ReS2 as a model for the hydrogen evolution reaction (HER), we uncover that intrinsic charge engineering has an auto-optimizing effect on enhancing catalytic activity through regulating active electronic states. The experimental and theoretical results show that intrinsic charge compensation from S to Re-Re bonds could manipulate the active electronic states, allowing hydrogen to absorb the active sites neither strongly nor weakly. Two types of S sites exhibit the optimal hydrogen adsorption free energies (Delta G(H*)) of 0.016 and 0.061 eV, which are the closest to zero corresponding to the highest HER activity. This auto-optimization via charge engineering is further demonstrated by higher turnover frequency per sulfur atom of 1-10 s(-1) and lower overpotential of -147 mV cm(-2) TMDs through multiscale activation and optimization. This work opens an avenue in designing extensive active catalysts through intrinsic charge engineering strategy.
学科主题	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000433404500044
资助机构	The authors acknowledge financial support from the National Key Research and Development Program of China (2016YFB0700204), the National Natural Science Foundation of China (51502327, 51602332, 51432010, 21573272, 51702345), and One Hundred Talent Plan of Chinese Academy of Sciences. J.Z. and Z.L. are grateful for the financial support from the Singapore National Research Foundation under NRF RF Award No. NRF-RF2013-08 and MOE Tier 2 Grant MOE2016-T2-1-131. J.L. and K.S. acknowledge JST-ACCEL and JSPS KAKENHI (JP16H06333, JP25107003, and P16382) for financial support. ; The authors acknowledge financial support from the National Key Research and Development Program of China (2016YFB0700204), the National Natural Science Foundation of China (51502327, 51602332, 51432010, 21573272, 51702345), and One Hundred Talent Plan of Chinese Academy of Sciences. J.Z. and Z.L. are grateful for the financial support from the Singapore National Research Foundation under NRF RF Award No. NRF-RF2013-08 and MOE Tier 2 Grant MOE2016-T2-1-131. J.L. and K.S. acknowledge JST-ACCEL and JSPS KAKENHI (JP16H06333, JP25107003, and P16382) for financial support.
内容类型	期刊论文
源URL	[http://ir.sic.ac.cn/handle/331005/24940]
专题	中国科学院上海硅酸盐研究所
作者单位	1.Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, 1295 Dingxi Rd, Shanghai 200050, Peoples R China 2.Nanyang Technol Univ, Sch Mat Sci & Engn, Ctr Programmable Mat, Singapore 639798, Singapore 3.Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058565, Japan 4.Shanghai Inst Mat Genome, 99 Shangda Rd, Shanghai 200444, Peoples R China
推荐引用方式 GB/T 7714	Zhou, Yao,Song, Erhong,Zhou, Jiadong,et al. Auto-optimizing Hydrogen Evolution Catalytic Activity of ReS2 through Intrinsic Charge Engineering[J]. ACS NANO,2018,12(5):4486, 4493.
APA	Zhou, Yao.,Song, Erhong.,Zhou, Jiadong.,Lin, Junhao.,Ma, Ruguang.,...&Liu, Jianjun.(2018).Auto-optimizing Hydrogen Evolution Catalytic Activity of ReS2 through Intrinsic Charge Engineering.ACS NANO,12(5),4486.
MLA	Zhou, Yao,et al."Auto-optimizing Hydrogen Evolution Catalytic Activity of ReS2 through Intrinsic Charge Engineering".ACS NANO 12.5(2018):4486.