ccu掺杂银基乙烯环氧化催化剂的设计

IF 1.2 4区 化学 Q4 PHYSICS, ATOMIC, MOLECULAR & CHEMICAL Chinese Journal of Chemical Physics Pub Date : 2022-08-01 DOI:10.1063/1674-0068/cjcp2112246
Q. Wen, Haoxiang Xu, Yang Nan, Yuan Xie, D. Cheng
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引用次数: 0

摘要

我们最近的理论研究已经筛选出了ccu掺杂的银基乙烯环氧化催化剂[ACS catalal . 11, 3371(2021)]。理论结果是基于表面模拟的,而实际反应过程中Ag催化剂是颗粒状的。本文结合密度泛函理论(DFT)、Wulff结构理论和微动力学分析,在粒子模型下研究了银催化剂的催化性能。结果表明,ccu掺杂的Ag催化剂在选择性和活性方面都优于纯Ag催化剂,并通过实验验证进一步证明了这一点。表征分析发现,Cu和Cs掺杂均促进了颗粒的生长和弥散,形成了富晶界的Ag颗粒。此外,cu还能促进催化剂表面亲电原子氧的生成,有利于环氧乙烷的生成和解吸。我们的工作为理论与实验相结合的催化剂设计提供了案例研究。
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Design of CuCs-doped Ag-based catalyst for ethylene epoxidation
Our recent theoretical studies have screened out CuCs-doped Ag-based promising catalysts for ethylene epoxidation [ACS Catal. 11, 3371 (2021)]. The theoretical results were based on surface modeling, while in the actual reaction process Ag catalysts are particle shaped. In this work, we combine density functional theory (DFT), Wulff construction theory, and micro kinetic analysis to study the catalytic performance of Ag catalysts at the particle model. It demonstrates that the CuCs-doped Ag catalysts are superior to pure Ag catalysts in terms of selectivity and activity, which is further proved by experimental validation. The characterization analysis finds that both Cu and Cs dopant promote particle growth as well as particle dispersion, resulting in a grain boundary-rich Ag particle. Besides, CuCs also facilitate electrophilic atomic oxygen formation on catalyst surface, which is benefitial for ethylene oxide formation and desorption. Our work provides a case study for catalyst design by combining theory and experiment.
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来源期刊
Chinese Journal of Chemical Physics
Chinese Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
1.90
自引率
10.00%
发文量
2763
审稿时长
3 months
期刊介绍: Chinese Journal of Chemical Physics (CJCP) aims to bridge atomic and molecular level research in broad scope for disciplines in chemistry, physics, material science and life sciences, including the following: Theoretical Methods, Algorithms, Statistical and Quantum Chemistry Gas Phase Dynamics and Structure: Spectroscopy, Molecular Interactions, Scattering, Photochemistry Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation Processes Surfaces, Interfaces, Single Molecules, Materials and Nanosciences Polymers, Biopolymers, and Complex Systems Other related topics
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