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单碳空位捕获原子铂用于析氢催化
作者:小柯机器人 发布时间:2022/1/12 10:22:03

吉林大学姚向东团队设计了单碳空位捕获原子铂用于析氢催化。相关研究成果于2022年1月7日发表在《美国化学会杂志》。

铂原子(Pt)的配位构型一直被认为是析氢反应(HER)中具有高本征活性的活性中心。

该文中,研究人员有意在碳基体(缺陷石墨烯)中合成单个空位,该空位可以捕获原子Pt以形成Pt–C3构型,从而使其在酸性和碱性溶液中都具有极高的反应活性。Pt–C3位点的固有活性在100 mV时的转换频率(TOF)分别为26.41 s–1和26.05A g–1,结果表明,最佳配位Pt–C3具有更强的电子俘获能力和更低的吉布斯自由能差(ΔG),从而促进吸附H+的还原和H2解吸的加速,从而显示出非凡的活动能力。

该工作为色散原子Pt在缺陷C矩阵中独特的配位结构提供了新的见解,从而提高了其性能。

附:英文原文

Title: Single Carbon Vacancy Traps Atomic Platinum for Hydrogen Evolution Catalysis

Author: Qin Yang, Hanxuan Liu, Pei Yuan, Yi Jia, Linzhou Zhuang, Hongwei Zhang, Xuecheng Yan, Guihao Liu, Yufei Zhao, Jizi Liu, Shiqiang Wei, Li Song, Qilong Wu, Bingqing Ge, Longzhou Zhang, Kang Wang, Xin Wang, Chun-Ran Chang, Xiangdong Yao

Issue&Volume: January 7, 2022

Abstract: 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–C3 configuration, which gives exceptionally high reactivity for HER in both acidic and alkaline solutions. The intrinsic activity of Pt–C3 site is valued with a turnover frequency (TOF) of 26.41 s–1 and mass activity of 26.05 A g–1 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–C3 has a stronger electron-capture ability and lower Gibbs free energy difference (ΔG), resulting in promoting the reduction of adsorbed H+ and the acceleration of H2 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.

DOI: 10.1021/jacs.1c10814

Source: https://pubs.acs.org/doi/10.1021/jacs.1c10814

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000