Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution

被引:542
作者
Luo, Zhaoyan [1 ,2 ]
Ouyang, Yixin [3 ]
Zhang, Hao [4 ]
Xiao, Meiling [1 ]
Ge, Junjie [1 ]
Jiang, Zheng [4 ]
Wang, Jinlan [3 ,5 ]
Tang, Daiming [6 ]
Cao, Xinzhong [7 ]
Liu, Changpeng [1 ]
Xing, Wei [1 ]
机构
[1] Chinese Acad Sci, State Key Lab Electroanalyt Chem, Jilin Prov Key Lab Low Carbon Chem Power, Changchun Inst Appl Chem, Changchun 130022, Jilin, Peoples R China
[2] Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China
[3] Southeast Univ, Sch Phys, Nanjing 211189, Jiangsu, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[5] Hunan Normal Univ, SICQEA, Changsha 410081, Hunan, Peoples R China
[6] Natl Inst Mat Sci, Namiki 1-1, Tsukuba, Ibaraki 3050044, Japan
[7] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
INITIO MOLECULAR-DYNAMICS; GENERALIZED GRADIENT APPROXIMATION; ACTIVE EDGE SITES; MOLYBDENUM-DISULFIDE; SULFUR VACANCIES; PHASE; TRANSITION; NANOSHEETS; MONOLAYER; CATALYST;
D O I
10.1038/s41467-018-04501-4
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Lacking strategies to simultaneously address the intrinsic activity, site density, electrical transport, and stability problems of chalcogels is restricting their application in catalytic hydrogen production. Herein, we resolve these challenges concurrently through chemically activating the molybdenum disulfide (MoS2) surface basal plane by doping with a low content of atomic palladium using a spontaneous interfacial redox technique. Palladium substitution occurs at the molybdenum site, simultaneously introducing sulfur vacancy and converting the 2H into the stabilized 1T structure. Theoretical calculations demonstrate the sulfur atoms next to the palladium sites exhibit low hydrogen adsorption energy at -0.02 eV. The final MoS2 doped with only 1wt% of palladium demonstrates exchange current density of 805 mu A cm(-2) and 78 mV overpotential at 10 mA cm(-2), accompanied by a good stability. The combined advantages of our surface activating technique open the possibility of manipulating the catalytic performance of MoS2 to rival platinum.
引用
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页数:8
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