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

Shengjue Deng; Mi Luo; Changzhi Ai; Yan Zhang; Bo Liu; Lei Huang; Zheng Jiang; Qinghua Zhang; Lin Gu; Shiwei Lin; Xiuli Wang; Lei Yu; Jianguo Wen; Jiaao Wang; Guoxiang Pan; Xinhui Xia; Jiangping Tu

doi:10.1002/anie.201909698

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

Angew Chem Int Ed Engl. 2019 Nov 4;58(45):16289-16296. doi: 10.1002/anie.201909698. Epub 2019 Sep 24.

Authors

Shengjue Deng¹, Mi Luo², Changzhi Ai³, Yan Zhang¹, Bo Liu¹, Lei Huang¹, Zheng Jiang², Qinghua Zhang⁴, Lin Gu⁴, Shiwei Lin³, Xiuli Wang¹, Lei Yu⁵, Jianguo Wen⁵, Jiaao Wang⁶, Guoxiang Pan⁷, Xinhui Xia¹, Jiangping Tu¹

Affiliations

¹ State Key Laboratory of Silicon Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, Department of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
² Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201210, P. R. China.
³ State Key Laboratory of Marine Resource Utilization, in South China Sea, Hainan University, Haikou, 570228, P. R. China.
⁴ Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
⁵ Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL, 60439, USA.
⁶ School of Material Science and Engineering, University of Jinan, Jinan, 250022, China.
⁷ Department of Materials Chemistry, Huzhou University, Huzhou, 313000, P. R. China.

PMID: 31487116
DOI: 10.1002/anie.201909698

Abstract

A synergistic N doping plus PO₄ ^3- 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 PO₄ ^3- 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,PO₄ ^3- )-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,PO₄ ^3- )-MoS₂ /VG electrode shows excellent HER performance with a lower Tafel slope and overpotential than N-MoS₂ /VG, PO₄ ^3- -MoS₂ /VG counterparts, and other Mo-base catalysts in the literature.

Keywords: doping-intercalation; hydrogen evolution reaction; molybdenum sulfide; nitrogen; phosphate.

Publication types

Review

Grants and funding

51728204, 51772272, 51502263/National Natural Science Foundation of China