Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction

Yin, Ying; Zhang, Yumin; Gao, Tangling; Yao, Tai; Zhang, Xinghong; Han, Jiecai; Wang, Xianjie; Zhang, Zhihua; Xu, Ping; Zhang, Peng; Cao, Xingzhong; Song, Bo; Jin, Song

doi:10.1002/adma.201700311

Synergistic Phase and Disorder Engineering in 1T‐MoSe ₂ Nanosheets for Enhanced Hydrogen‐Evolution Reaction

Journal Article · Fri May 19 00:00:00 EDT 2017 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201700311· OSTI ID:1400842

Yin, Ying ^[1]; Zhang, Yumin ^[1]; Gao, Tangling ^[2]; Yao, Tai ^[3]; Zhang, Xinghong ^[1]; Han, Jiecai ^[1]; Wang, Xianjie ^[3]; Zhang, Zhihua ^[4]; Xu, Ping ^[5]; Zhang, Peng ^[6]; Cao, Xingzhong ^[6]; ^[3]; ^[7]

Centre for Composite Materials and Structures Harbin Institute of Technology Harbin 150001 China
Institute of Petrochemistry Heilongjiang Academy of Sciences Harbin 150040 China
Academy of Fundamental and Interdisciplinary Sciences Department of Physics Harbin Institute of Technology Harbin 150001 China
School of Materials Science and Engineering Dalian Jiaotong University Dalian 116028 China
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 China
Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China
Department of Chemistry University of Wisconsin–Madison 1101 University Avenue Madison WI 53706 USA

MoSe ₂ is a promising earth‐abundant electrocatalyst for the hydrogen‐evolution reaction (HER), even though it has received much less attention among the layered dichalcogenide (MX ₂ ) materials than MoS ₂ so far. Here, a novel hydrothermal‐synthesis strategy is presented to achieve simultaneous and synergistic modulation of crystal phase and disorder in partially crystallized 1T‐MoSe ₂ nanosheets to dramatically enhance their HER catalytic activity. Careful structural characterization and defect characterization using positron annihilation lifetime spectroscopy correlated with electrochemical measurements show that the formation of the 1T phase under a large excess of the NaBH ₄ reductant during synthesis can effectively improve the intrinsic activity and conductivity, and the disordered structure from a lower reaction temperature can provide abundant unsaturated defects as active sites. Such synergistic effects lead to superior HER catalytic activity with an overpotential of 152 mV versus reversible hydrogen electrode (RHE) for the electrocatalytic current density of j = −10 mA cm ⁻² , and a Tafel slope of 52 mV dec ⁻¹ . This work paves a new pathway for improving the catalytic activity of MoSe ₂ and generally MX ₂ ‐based electrocatalysts via a synergistic modulation strategy.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-09ER46664

OSTI ID:: 1400842

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 28 Vol. 29; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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