Yang Qin, Liu Hanxuan, Yuan Pei, Jia Yi, Zhuang Linzhou, Zhang Hongwei, Yan Xuecheng, Liu Guihao, Zhao Yufei, Liu Jizi, Wei Shiqiang, Song Li, Wu Qilong, Ge Bingqing, Zhang Longzhou, Wang Kang, Wang Xin, Chang Chun-Ran, Yao Xiangdong
College of Chemical Engineering, Fuzhou University, Fuzhou 350002, P.R. China.
School of Environment and Science, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan, Queensland 4111, Australia.
J Am Chem Soc. 2022 Feb 9;144(5):2171-2178. doi: 10.1021/jacs.1c10814. Epub 2022 Jan 7.
The coordinated configuration of atomic platinum (Pt) has always been identified as an active site with high intrinsic activity for hydrogen evolution reaction (HER). Herein, we purposely synthesize single vacancies in a carbon matrix (defective graphene) that can trap atomic Pt to form the Pt-C configuration, which gives exceptionally high reactivity for HER in both acidic and alkaline solutions. The intrinsic activity of Pt-C site is valued with a turnover frequency (TOF) of 26.41 s and mass activity of 26.05 A g at 100 mV, respectively, which are both nearly 18 times higher than those of commercial 20 wt % Pt/C. It is revealed that the optimal coordination Pt-C has a stronger electron-capture ability and lower Gibbs free energy difference (Δ), resulting in promoting the reduction of adsorbed H and the acceleration of H desorption, thus exhibiting the extraordinary HER activity. This work provides a new insight on the unique coordinated configuration of dispersive atomic Pt in defective C matrix for superior HER performance.
原子铂（Pt）的配位构型一直被认为是析氢反应（HER）具有高本征活性的活性位点。在此，我们特意在碳基质（缺陷石墨烯）中合成单空位，其可以捕获原子Pt形成Pt-C构型，这在酸性和碱性溶液中均赋予HER极高的反应活性。Pt-C位点的本征活性分别以26.41 s的转换频率（TOF）和100 mV下26.05 A g的质量活性来衡量，两者均比商业20 wt% Pt/C高出近18倍。研究表明，最佳配位的Pt-C具有更强的电子捕获能力和更低的吉布斯自由能差（Δ），从而促进吸附H的还原和H脱附的加速，进而展现出非凡的HER活性。这项工作为缺陷C基质中分散原子Pt的独特配位构型实现优异的HER性能提供了新的见解。
