Metallic W/WO(2) solid-acid catalyst boosts hydrogen evolution reaction in alkaline electrolyte.
Metallic W/WO(2) solid-acid catalyst boosts hydrogen evolution reaction in alkaline electrolyte.
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DOI：
10.1038/s41467-023-41097-w
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发表时间：
2023-09-02
影响因子：
16.6
通讯作者：
Cui, Yi
中科院分区：
文献类型：
--
作者：
Chen, Zhigang;Gong, Wenbin;Wang, Juan;Hou, Shuang;Yang, Guang;Zhu, Chengfeng;Fan, Xiyue;Li, Yifan;Gao, Rui;Cui, Yi
与酸中相比，碱性析氢反应过程中有效质子的缺乏严重降低了反应活性，通过调节质子在催化剂表面的覆盖度和化学环境可以有效地促进碱性析氢反应。然而，由于贵金属原子和质子之间吸引人的电子相互作用，通过质子转移的活性位点的循环在很大程度上取决于贵金属催化剂的利用。在此，用作高效固体酸催化剂的全非贵金属W/WO 2金属异质结构表现出显著的析氢反应性能，在-10 mA/cm 2下具有-35 mV的超低过电位和小的塔菲尔斜率（-34 mV/dec），以及在碱性电解质中在-10和-50 mA/cm 2的电流密度下的长期制氢耐久性（>50 h）。多个原位和非原位光谱表征结合第一性原理密度泛函理论计算发现，在超低过电位下，W/WO 2固体酸催化剂可构建动态质子富集表面，使W/WO 2催化碱性制氢遵循两个相邻质子重组成氢分子的快速动力学Volmer-Tafel途径.我们的策略，固体酸催化剂和利用多种光谱表征可能会提供一个有趣的路线，设计先进的全非贵金属催化体系，以提高析氢反应性能在碱性电解质。贵金属的高成本和低丰度极大地限制了电化学制氢的实际应用。在这里，作者在金属二氧化钨纳米棒上制备了超小的钨纳米颗粒，并表现出优异的碱性析氢反应活性。
The lack of available protons severely lowers the activity of alkaline hydrogen evolution reaction process than that in acids, which can be efficiently accelerated by tuning the coverage and chemical environment of protons on catalyst surface. However, the cycling of active sites by proton transfer is largely dependent on the utilization of noble metal catalysts because of the appealing electronic interaction between noble metal atoms and protons. Herein, an all-non-noble W/WO2 metallic heterostructure serving as an efficient solid-acid catalyst exhibits remarkable hydrogen evolution reaction performance with an ultra-low overpotential of −35 mV at −10 mA/cm2 and a small Tafel slope (−34 mV/dec), as well as long-term durability of hydrogen production (>50 h) at current densities of −10 and −50 mA/cm2 in alkaline electrolyte. Multiple in situ and ex situ spectroscopy characterizations combining with first-principle density functional theory calculations discover that a dynamic proton-concentrated surface can be constructed on W/WO2 solid-acid catalyst under ultra-low overpotentials, which enables W/WO2 catalyzing alkaline hydrogen production to follow a kinetically fast Volmer-Tafel pathway with two neighboring protons recombining into a hydrogen molecule. Our strategy of solid-acid catalyst and utilization of multiple spectroscopy characterizations may provide an interesting route for designing advanced all-non-noble catalytic system towards boosting hydrogen evolution reaction performance in alkaline electrolyte. The high cost and low abundance of noble metals largely restrict practical applications for electrochemical hydrogen production. Here, the authors prepare ultrasmall tungsten nanoparticles on metallic tungsten dioxide nanorods and demonstrate excellent activities for the alkaline hydrogen evolution reaction.
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