摘要
The underpotential adsorption of hydrogen (HUPD) is one of the most attractive fields in surface electrochemistry and electrocatalysis. In this work, the hydrogen adsorption on polycrystalline platinum electrode experimentally as well as on single crystal Pt(110) and Pt(100) electrode theoretically were studied. The effect of forced convection on the adsorption and desorption process of hydrogen was studied through adjusting the sampling rate of the microporous sampler closing to the surface of the platinum electrode immersed in dilute sulfuric acid solution. The relationship between HUPD and surface structure sensitivity was built quantitively. The DFT simulation shows that the adsorption strength of hydrogen on Pt(100), due to the lower adsorption energy, is weaker than that on Pt(110). Moreover, the bridged position of hydrogen on Pt(100) and the short-range bridged position on Pt(110) were found to be the optimal adsorption sites. The study of forced convection on the electrode surface promotes the HUPD research from static process to a convective mode and also provides a new strategy to investigate the hydrogen adsorption in solution.
The underpotential adsorption of hydrogen(HUPD)is one of the most attractive fields in surface electrochemistry and electrocatalysis.In this work,the hydrogen adsorption on polycrystalline platinum electrode experimentally as well as on single crystal Pt(110)and Pt(100)electrode theoretically were studied.The effect of forced convection on the adsorption and desorption process of hydrogen was studied through adjusting the sampling rate of the microporous sampler closing to the surface of the platinum electrode immersed in dilute sulfuric acid solutio n.The relationship between HUPD and surface structure sensitivity was built quantitively.The DFT simulation shows that the adsorption strength of hydrogen on Pt(100),due to the lower adsorption energy,is weaker than that on Pt(110).Moreover,the bridged position of hydro gen on Pt(100)and the sho rt-range bridged position on Pt(110)we re found to be the optimal adsorption sites.The study of fo rced convection on the electrode surface pro motes the HUPD research from static process to a convective mode and also provides a new strategy to investigate the hydrogen adsorption in solution.
基金
the National Natural Science Foundation of China (No. 21773304)
the Fundamental Research Funds for the Central Universities(No. 2015XKZD09)
the Natural Science Foundation of Jiangsu Province(No. BK20160240)
the Research Innovation Project for College Graduates of Jiangsu Province (No. KYLX16_0549)
the Research Foundation Project of Zaozhuang University (No. 2017YB24)
Doctoral Foundation Program of Zaozhuang University(No.2018BS060,102201702)
