Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution

Nature Communications
Yichao HuangJing Gu

Abstract

Engineering catalytic sites at the atomic level provides an opportunity to understand the catalyst's active sites, which is vital to the development of improved catalysts. Here we show a reliable and tunable polyoxometalate template-based synthetic strategy to atomically engineer metal doping sites onto metallic 1T-MoS2, using Anderson-type polyoxometalates as precursors. Benefiting from engineering nickel and oxygen atoms, the optimized electrocatalyst shows great enhancement in the hydrogen evolution reaction with a positive onset potential of ~ 0 V and a low overpotential of -46 mV in alkaline electrolyte, comparable to platinum-based catalysts. First-principles calculations reveal co-doping nickel and oxygen into 1T-MoS2 assists the process of water dissociation and hydrogen generation from their intermediate states. This research will expand on the ability to improve the activities of various catalysts by precisely engineering atomic activation sites to achieve significant electronic modulations and improve atomic utilization efficiencies.

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Citations

Aug 2, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Lang PeiZhigang Zou
Sep 13, 2019·Small·Zhi-Wen GaoLawrence Yoon Suk Lee
Dec 7, 2019·Chemical Communications : Chem Comm·Ori Geuli, Daniel Mandler
Aug 11, 2020·Advanced Functional Materials·Yuanhui SunLijun Zhang
Dec 2, 2020·Proceedings of the National Academy of Sciences of the United States of America·Daoping HeRyuhei Nakamura
Apr 24, 2021·Nanoscale·Pingfan WuZicheng Xiao
Jun 5, 2021·Advanced Science·Frederick Osei-Tutu Agyapong-FordjourKi Kang Kim
Jun 15, 2021·Chemical Science·Otega A EjegbavwoNatalia B Shustova
Jul 27, 2021·Chemical Society Reviews·An ZhangJie Zeng
Sep 26, 2019·ACS Applied Materials & Interfaces·Duc Anh NguyenMun Seok Jeong
Apr 1, 2020·ACS Omega·Sadegh Imani YengejehYun Wang
Nov 12, 2019·The Journal of Physical Chemistry Letters·Liping YuQimin Yan

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Methods Mentioned

BETA
infrared spectroscopy
scanning electron microscopy
transmission electron microscopy
X-ray

Software Mentioned

USTCXAFS
FEFF
DigitalMicrograph
XPSPEAK41
IFEFFIT

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