Comprehensive understanding of ethylene epoxidation on copper catalysts: a microkinetic study with coverage effects

doi:10.1039/d4cy00617h

	Comprehensive understanding of ethylene epoxidation on copper catalysts: a microkinetic study with coverage effects
	Wang, Zhuozheng 1,2,3; Xie, Wenbo2,3 ; Xu, Yarong 4; Han, Yulan 3; Xu, Jiayan 3; Hu, P.2,3
	2024
发表期刊	CATALYSIS SCIENCE AND TECHNOLOGY (IF:4.4[JCR-2023],4.7[5-Year])
ISSN	2044-4753
EISSN	2044-4761
卷号	14 期号:18 页码:5291-5303
发表状态	已发表
DOI	10.1039/d4cy00617h
摘要	Ethylene epoxidation is one of the fundamental industrial reactions, garnering extensive theoretical and experimental studies. While silver has traditionally been the catalyst of choice for this reaction, copper has received comparatively little attention. In this study, we apply a coverage-dependent microkinetic modeling to quantitatively investigate ethylene epoxidation on Cu(111), serving as a model system to study the intrinsic activity and selectivity of Cu catalysts. The coverage-dependent simulation takes into account both self and cross-interactions of adsorbates, as well as the coverage effects on the transition states of each elementary step. In contrast, the coverage-independent modeling is conducted without considering coverage effects. We observe that the coverage-dependent modelling reveals the Cu(111) surface with coverage exceeding 30% oxygen atoms with a high turnover frequency (log(TOF) = 2.65) at 500 K. In contrast, the coverage-independent results indicate the Cu(111) surface being completely covered by oxygen atoms, leading to detrimental poisoning effects (log(TOF) = −2.47). We show that the EO selectivity on Cu(111) can be at a high level of 80% under all studied conditions in contrast to only ∼40% EO selectivity on Ag(111). Detailed structural analyses unveil the fundamental reasons why Cu catalysts are more selective for ethylene epoxidation. Furthermore, we suggest that reducing temperature and increasing oxygen pressure can effectively improve EO selectivity for industrial ethylene epoxidation. © 2024 The Royal Society of Chemistry.
关键词	Catalyst selectivity Ethylene Oxygen Copper catalyst Cu catalyst Cu catalysts Cu-catalysts Ethylene epoxidation Industrial reactions Microkinetics Oxygen atom Turnover frequency ]+ catalyst
URL	查看原文
收录类别	EI ; SCI
语种	英语
资助项目	NSFC[92045303] ; NKRDPC[2021YFA1500700] ; UK national high-performance computing service ARCHER - EPSRC[EP/P022561/1] ; QUB Kelvin HPC service - ESPRC[EP/T022175/1] ; EPSRC[EP/P020194/1]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:001288430600001
出版者	Royal Society of Chemistry
EI入藏号	20243316885337
EI主题词	Copper
EI分类号	544.1 Copper ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.1 Organic Compounds
原始文献类型	Article in Press
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/411253
专题	物质科学与技术学院生物医学工程学院_PI研究组_胡鹏组物质科学与技术学院_PI研究组_胡培君组
通讯作者	Hu, P.
作者单位	1.PetroChina Petrochemical Research Institute, Beijing; 102206, China 2.School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Shanghai; 201210, China 3.School of Chemistry and Chemical Engineering, The Queen's University of Belfast, Belfast; BT9 5AG, United Kingdom 4.Research Institute of Urumqi Petrochemical Company, PetroChina Company Limited, Urumqi; 830019, China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Wang, Zhuozheng,Xie, Wenbo,Xu, Yarong,et al. Comprehensive understanding of ethylene epoxidation on copper catalysts: a microkinetic study with coverage effects[J]. CATALYSIS SCIENCE AND TECHNOLOGY,2024,14(18):5291-5303.
APA	Wang, Zhuozheng,Xie, Wenbo,Xu, Yarong,Han, Yulan,Xu, Jiayan,&Hu, P..(2024).Comprehensive understanding of ethylene epoxidation on copper catalysts: a microkinetic study with coverage effects.CATALYSIS SCIENCE AND TECHNOLOGY,14(18),5291-5303.
MLA	Wang, Zhuozheng,et al."Comprehensive understanding of ethylene epoxidation on copper catalysts: a microkinetic study with coverage effects".CATALYSIS SCIENCE AND TECHNOLOGY 14.18(2024):5291-5303.