钯
氢化钯
透射电子显微镜
原位
电化学
氢化物
材料科学
电子显微镜
衍射
化学
纳米技术
电极
金属
光学
催化作用
物理化学
有机化学
冶金
物理
作者
Ahmed Abdellah,Fatma Ismail,Oliver W. Siig,Jie Yang,Carmen M. Andrei,Liza‐Anastasia DiCecco,Amirhossein Rakhsha,Kholoud E. Salem,Kathryn Grandfield,Nabil Bassim,Robert W. Black,Georg Kastlunger,Leyla Soleymani,Drew Higgins
标识
DOI:10.1038/s41467-024-45096-3
摘要
Abstract Electrochemical conversion of CO 2 offers a sustainable route for producing fuels and chemicals. Pd-based catalysts are effective for converting CO 2 into formate at low overpotentials and CO/H 2 at high overpotentials, while undergoing poorly understood morphology and phase structure transformations under reaction conditions that impact performance. Herein, in-situ liquid-phase transmission electron microscopy and select area diffraction measurements are applied to track the morphology and Pd/PdH x phase interconversion under reaction conditions as a function of electrode potential. These studies identify the degradation mechanisms, including poisoning and physical structure changes, occurring in PdH x /Pd electrodes. Constant potential density functional theory calculations are used to probe the reaction mechanisms occurring on the PdH x structures observed under reaction conditions. Microkinetic modeling reveals that the intercalation of *H into Pd is essential for formate production. However, the change in electrochemical CO 2 conversion selectivity away from formate and towards CO/H 2 at increasing overpotentials is due to electrode potential dependent changes in the reaction energetics and not a consequence of morphology or phase structure changes.
科研通智能强力驱动
Strongly Powered by AbleSci AI