Chen Zhigang, Xu Yafeng, Ding Ding, Song Ge, Gan Xingxing, Li Hao, Wei Wei, Chen Jian, Li Zhiyun, Gong Zhongmiao, Dong Xiaoming, Zhu Chengfeng, Yang Nana, Ma Jingyuan, Gao Rui, Luo Dan, Cong Shan, Wang Lu, Zhao Zhigang, Cui Yi
Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123, China.
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, Jiangsu, 215123, China.
Nat Commun. 2022 Feb 9;13(1):763. doi: 10.1038/s41467-022-28413-6.
Tungsten carbides, featured by their Pt-like electronic structure, have long been advocated as potential replacements for the benchmark Pt-group catalysts in hydrogen evolution reaction. However, tungsten-carbide catalysts usually exhibit poor alkaline HER performance because of the sluggish hydrogen desorption behavior and possible corrosion problem of tungsten atoms by the produced hydroxyl intermediates. Herein, we report the synthesis of tungsten atomic clusters anchored on P-doped carbon materials via a thermal-migration strategy using tungsten single atoms as the parent material, which is evidenced to have the most favorable Pt-like electronic structure by in-situ variable-temperature near ambient pressure X-ray photoelectron spectroscopy measurements. Accordingly, tungsten atomic clusters show markedly enhanced alkaline HER activity with an ultralow overpotential of 53 mV at 10 mA/cm and a Tafel slope as low as 38 mV/dec. These findings may provide a feasible route towards the rational design of atomic-cluster catalysts with high alkaline hydrogen evolution activity.
碳化钨具有类似铂的电子结构，长期以来一直被倡导作为析氢反应中基准铂族催化剂的潜在替代品。然而，碳化钨催化剂通常表现出较差的碱性析氢性能，这是由于氢脱附行为迟缓以及所产生的羟基中间体可能对钨原子造成腐蚀问题。在此，我们报道了通过以钨单原子为母体材料的热迁移策略合成锚定在P掺杂碳材料上的钨原子簇，原位变温近常压X射线光电子能谱测量证明其具有最有利的类似铂的电子结构。因此，钨原子簇表现出显著增强的碱性析氢活性，在10 mA/cm²时过电位低至53 mV，塔菲尔斜率低至38 mV/dec。这些发现可能为合理设计具有高碱性析氢活性的原子簇催化剂提供一条可行的途径。
