Synergistic Doping and Intercalation: Realizing Deep Phase Modulation on MoS2 Arrays for High-Efficiency Hydrogen Evolution Reaction

被引:221
作者
Deng, Shengjue [1 ,2 ]
Luo, Mi [3 ]
Ai, Changzhi [4 ]
Zhang, Yan [1 ,2 ]
Liu, Bo [1 ,2 ]
Huang, Lei [1 ,2 ]
Jiang, Zheng [3 ]
Zhang, Qinghua [5 ]
Gu, Lin [5 ]
Lin, Shiwei [4 ]
Wang, Xiuli [1 ,2 ]
Yu, Lei [6 ]
Wen, Jianguo [6 ]
Wang, Jiaao [7 ]
Pan, Guoxiang [8 ]
Xia, Xinhui [1 ,2 ]
Tu, Jiangping [1 ,2 ]
机构
[1] Zhejiang Univ, Key Lab Adv Mat & Applicat Batteries Zhejiang Pro, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China
[2] Zhejiang Univ, Dept Mat Sci & Engn, Hangzhou 310027, Zhejiang, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China
[4] Hainan Univ, State Key Lab Marine Resource Utilizat South Chin, Haikou 570228, Hainan, Peoples R China
[5] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
[6] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA
[7] Univ Jinan, Sch Mat Sci & Engn, Jinan 250022, Shandong, Peoples R China
[8] Huzhou Univ, Dept Mat Chem, Huzhou 313000, Peoples R China
基金
中国国家自然科学基金;
关键词
doping-intercalation; hydrogen evolution reaction; molybdenum sulfide; nitrogen; phosphate; NANOSHEETS; TRANSITION; HETEROSTRUCTURES; SPECTROSCOPY; CARBON;
D O I
10.1002/anie.201909698
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A synergistic N doping plus PO43- intercalation strategy is used to induce high conversion (ca. 41 %) of 2H-MoS2 into 1T-MoS2, which is much higher than single N doping (ca. 28 %) or single PO43- intercalation (ca. 10 %). A scattering mechanism is proposed to illustrate the synergistic phase transformation from the 2H to the 1T phase, which was confirmed by synchrotron radiation and spherical aberration TEM. To further enhance reaction kinetics, the designed (N,PO43-)-MoS2 nanosheets are combined with conductive vertical graphene (VG) skeleton forming binder-free arrays for high-efficiency hydrogen evolution reaction (HER). Owing to the decreased band gap, lower d-band center, and smaller hydrogen adsorption/desorption energy, the designed (N,PO43-)-MoS2/VG electrode shows excellent HER performance with a lower Tafel slope and overpotential than N-MoS2/VG, PO43--MoS2/VG counterparts, and other Mo-base catalysts in the literature.
引用
收藏
页码:16289 / 16296
页数:8
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