物理化学学报2025，Vol.41Issue(9)：97-108,12.DOI:10.1016/j.actphy.2025.100100
单原子Pd促进的Cu催化剂用于乙醇脱氢
Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation
摘要
Abstract
Ethanol dehydrogenation is a vital elementary step in ethanol upgrading,for which Cu-based alloy catalysts are the most promising candidates.Nevertheless,elucidating the underlying reasons for the synergistic effect between alloying components and host metals remains challenging due to the intrinsic structural complexity and dynamic evolution of alloy catalysts under operational conditions.Herein,single-atom Pd modified Cu-MFI catalysts with well-defined structures were designed for ethanol dehydrogenation to acetaldehyde and hydrogen.Comprehensive characterizations using aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(AC-HAADF-STEM),X-ray absorption spectroscopy(XAS),X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations revealed that Pd atoms are isolated by surrounding Cu atoms with a coordination number of 9-10,forming-0.36e charged single-atom sites and being uniformly dispersed on the surface of Cu catalysts.The newly generated Pdδ-and Cuδ+sites synergistically reduced the activation energy barrier for C―H bond cleavage in ethanol.These sites simultaneously enhanced hydrogen adsorption and H―H bond coupling,leading to improved ethanol conversion and acetaldehyde productivity over Pd/Cu-MFI catalysts.关键词
乙醇/脱氢/Pd-Cu单原子催化剂/电子转移/氢Key words
Ethanol/Dehydrogenation/Pd-Cu single-atom catalyst/Electron transfer/Hydrogen分类
化学化工引用本文复制引用
冯乐乐,白雪莹,庞纪峰,曹宏晨,刘晓艳,罗文豪,杨小峰,吴鹏飞,郑明远..单原子Pd促进的Cu催化剂用于乙醇脱氢[J].物理化学学报,2025,41(9):97-108,12.基金项目
This work was supported by the National Science Foundation of China(22378383,22279115)and the NSFC Center for Single-Atom Catalysis(22388102). 国家自然科学基金(22378383,22279115)及"单原子催化"基础科学中心(22388102)资助. （22378383,22279115）
