Boosting Hydrogen Evolution Reaction Activity of Amorphous Molybdenum Sulfide Under High Currents Via Preferential Electron Filling Induced by Tungsten Doping. Issue 27 (25th July 2022)

• Record Type: Journal Article
• Authors: Zhang, Dai; Wang, Feilong; Zhao, Wenqi; Cui, Minghui; Fan, Xueliang; Liang, Rongqing; Ou, Qiongrong; Zhang, Shuyu
• Is Part Of: Advanced materials interfaces. Volume 9:Issue 27(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-07-25
• Subjects: amorphous molybdenum tungsten sulfide -- amorphous transition‐metal sulfides -- density functional theory -- high current density -- hydrogen evolution reaction -- plasma treatment; Materials science -- Periodicals; 620.11
• DOI: 10.1002/advs.202202445
• Languages: English
• ISSNs: 2196-7350

Abstract

Abstract: 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‐MoWSx /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‐MoWSx /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 MoS2 ‐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 positive Δ 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. Abstract : This work describes a facile method for synthesizing amorphous molybdenum tungsten sulfide/nitrogen‐doped reduced graphene oxide nanocomposites toward efficient high‐current‐density hydrogen evolution reactions (HER). Density functional theory (DFT) calculations prove that 2S 2 − can be used to maintain high activity with electron injection and the introduction of tungsten tends to induce a closer‐to‐zero positive Δ G H * ${\Delta}{G}_{{\mathrm{H}}^{\ast}}$ under high current densities.