
近日,华南理工大学沈葵团队研究了用于高效和稳健碱析氢的原子镍氮化钨镜像对称纳米阵列网络。这一研究成果于2025年11月4日发表在《德国应用化学》杂志上。
碱性高效析氢反应电催化剂的发展对于未来阴离子交换膜水电解技术的应用至关重要。
研究组报道了一种新型杂原子诱导策略,可在碳布上构建镍掺杂三氧化钨的镜像对称纳米阵列网络,并据此设计出相应的新型原子级镍掺入氮氧化钨电催化剂用于碱性析氢反应。值得注意的是,该镍-氮氧化钨催化剂展现出高活性(-10 mA cm-2电流密度下过电位仅-35 mV)、小塔菲尔斜率(32 mV dec-1)及卓越的稳定性(-1.0 A cm-2电流密度下持续运行超过1200小时),是目前性能最优异的钨基碱性析氢电催化剂。
多种光谱表征表明,镍-氮氧化钨对强吸附性OH-/H2O基团具有高反应活性,可原位形成具有布朗斯特酸性的晶格羟基物种。研究组首次揭示该类羟基物种可作为介体,将金属-氢中间体的生成路径从传统分步模式转变为协同质子-电子转移模式,从而突破缺质子碱性环境中pH依赖性的限制。进一步同位素实验证实,表面介导的H-H耦合过程可在原子级W-Ni单元上高效加速,使镍-氮氧化钨催化剂能够通过动力学更优的新型协同质子-电子转移-塔菲尔路径实现碱性析氢反应。
附:英文原文
Title: Mirror-Symmetric Nanoarray Networks of Atomic Ni-Incorporated Tungsten Oxynitride for Efficient and Robust Alkaline Hydrogen Evolution
Author: Hongchuan Fu, Yucheng Wu, Li Wang, Ze Qin, Liyu Chen, Yingwei Li, Kui Shen
Issue&Volume: 2025-11-04
Abstract: The development of alkali-efficient hydrogen evolution reaction (HER) electrocatalysts is essential for future deployment of anion-exchange membrane water electrolysis technology. Herein, we report a novel heteroatom-induced strategy to construct the mirror-symmetric nanoarray networks of Ni-doped WO3 on carbon cloth and design a corresponding new type of atomic Ni-incorporated tungsten oxynitride (Ni-WNO) electrocatalyst for alkaline HER. Impressively, the Ni-WNO shows high activity (35 mV at 10 mA cm2), small Tafel slope (32 mV dec1) and excellent stability (>1200 h at 1.0 A cm2), representing the best-performing W-based electrocatalyst for alkaline HER. Multiple spectroscopy characterizations reveal that Ni-WNO is highly active for adsorbing aggressive OH/H2O groups, resulting in the in situ formation of lattice hydroxyl (i.e., WOH) species with Brnsted acidity, which, we disclose for the first time, can serve as a mediator to alter the generation of metalH intermediates from a conventional sequential to a concerted protonelectron transfer (CPET) pathway, thus breaking the pH-dependent limitations in proton-deficient alkalies. Further isotope experiments demonstrate that the surface-mediated HH coupling can be feasibly accelerated on atomic WNi units, thereby enabling Ni-WNO catalyzing alkaline HER via a new kinetically fast CPET–Tafel pathway.
DOI: 10.1002/anie.202518043
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202518043
Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx
