期刊
ADVANCED MATERIALS
卷 29, 期 28, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201700311
关键词
disorder; electrocatalysis; hydrogen-evolution reaction (HER); MoSe2; phase
类别
资金
- Major State Basic Search Program [2014CB46505]
- National Natural Science Foundation of China [51372056, 51472064, 51672057, 21471039, 21671047]
- Foundation for Innovative Research Groups of the National Natural Science Foundation of China [11421091]
- International Science & Technology Cooperation Program of China [2012DFR50020]
- Program for New Century Excellent Talents in University [NCET-13-0174]
- US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-09ER46664]
MoSe2 is a promising earth-abundant electrocatalyst for the hydrogen-evolution reaction (HER), even though it has received much less attention among the layered dichalcogenide (MX2) materials than MoS2 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-MoSe2 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 NaBH4 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 MoSe2 and generally MX2-based electrocatalysts via a synergistic modulation strategy.
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