Open AccessBoosting Hydrogen Evolution Reaction Activity of Amorphous Molybdenum Sulfide Under High Currents Via Preferential Electron Filling Induced by Tungsten Doping
Author(s) -
Zhang Dai,
Wang Feilong,
Zhao Wenqi,
Cui Minghui,
Fan Xueliang,
Liang Rongqing,
Ou Qiongrong,
Zhang Shuyu
Publication year - 2022
Publication title -
advanced science
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.388
H-Index - 100
ISSN - 2198-3844
DOI - 10.1002/advs.202202445
Subject(s) - overpotential , tungsten , materials science , catalysis , graphene , doping , molybdenum , density functional theory , amorphous solid , chemical engineering , hydrogen production , hydrogen , nanotechnology , chemistry , metallurgy , optoelectronics , computational chemistry , crystallography , organic chemistry , electrode , electrochemistry , engineering
The lack of highly efficient, durable, and cost‐effective electrocatalysts for the hydrogen evolution reaction (HER) working at high current densities poses a significant challenge for the large‐scale implementation of hydrogen production from renewable energy. Herein, amorphous molybdenum tungsten sulfide/nitrogen‐doped reduced graphene oxide nanocomposites (a‐MoWS x /N‐RGO) are synthesized by plasma treatment for use as high‐performance HER catalysts. By adjusting the plasma treatment duration and chemical composition, an optimal a‐MoWS x /N‐RGO catalyst is obtained, which exhibits a low overpotential of 348 mV at a current density of 1000 mA cm −2 and almost no decay after 24 h of working at this current density, outperforming commercial platinum/carbon (Pt/C) and previously reported heteroatom‐doped MoS 2 ‐based catalysts. Based on density functional theory (DFT) calculations, it is found that with a reasonable tungsten doping level, the catalytic active site (2S 2 − ) shows excellent catalytic performance working at high current densities because extra electrons preferentially fill at 2S 2 − . The introduction of tungsten tends to lower the electronic structure energy, resulting in a closer‐to‐zero positiveΔ G H ∗$\Delta {G}_{{{\rm{H}}}^{\rm{*}}}$ . Excessive tungsten introduction, however, can lead to structural damage and a worse HER performance under high current densities. The work provides a route towards rationally designing high‐performance catalysts for the HER at industrial‐level currents using earth‐abundant elements.