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How CO2 poisons La2O3 in an OCM catalytic reaction: A study by in situ XRD-MS and DFT
2021-04
发表期刊JOURNAL OF CATALYSIS (IF:6.5[JCR-2023],7.0[5-Year])
ISSN0021-9517
EISSN1090-2694
卷号396页码:202-214
发表状态已发表
DOI10.1016/j.jcat.2021.02.017
摘要

Oxidative coupling of methane (OCM) is a catalytic partial oxidation process that converts methane directly into more valuable C-2 products (ethane and ethylene). The mechanism related to selectivity and conversion is still not clear. Previous results suggested that the bulk structure change of the La2O3 catalyst is related to OCM activation performance. This work is focused on investigation of carbonates and the reaction products simultaneous formation over La2O3 catalyst utilizing coupled in situ XRDMS. Semi quantitative analysis clearly reveals a positive dependence between CO2 and C-2 products light-off temperature and the initial bulk La2O2CO3 concentration, indicating a strong correlation between carbonates and La2O3 catalyst poisoning. The activity of the La based catalyst is associated to its oxide form rather than to its oxycarbonate form. Based on operando results a two-step bulk La2O2CO3 decomposition model resulting in surface carbonates presenting on the catalyst surface between 500 degrees C and 800 degrees C is proposed. DFT calculations further confirm the proposed model and indicate surface carbonates do inhibit catalytic methane activation. It is concluded that CO32- species located in surface region of the catalyst operate as a direct La2O3 catalyst poison in the highly motivating OCM reaction. (C) 2021 Published by Elsevier Inc.

关键词OCM La2O3 Poison Coupled in situ XRD-MS DFT
收录类别SCIE ; EI
WOS研究方向Chemistry ; Engineering
WOS类目Chemistry, Physical ; Engineering, Chemical
WOS记录号WOS:000641071900003
出版者ACADEMIC PRESS INC ELSEVIER SCIENCE
原始文献类型Article
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文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/126712
专题物质科学与技术学院_博士生
物质科学与技术学院_PI研究组_杨永组
物质科学与技术学院_公共科研平台_分析测试平台
物质科学与技术学院_硕士生
通讯作者Yang, Yong
作者单位
1.Shanghai Tech Univ, Sch Phys Sci & Technol, 393 Huaxia Middle Rd, Shanghai 201210, Peoples R China;
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China;
3.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China;
4.Shell Global Solut Int BV, 5L-1031 CM Amsterdam, Netherlands;
5.Queens Univ Belfast, Sch Chem & Chem Engn, David Keir Bldg,Stranmillis Rd, Belfast BT9 5AG, Antrim, North Ireland
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
第一作者的第一单位物质科学与技术学院
推荐引用方式
GB/T 7714
Guan, Cairu,Yang, Yong,Pang, Yaoqi,et al. How CO2 poisons La2O3 in an OCM catalytic reaction: A study by in situ XRD-MS and DFT[J]. JOURNAL OF CATALYSIS,2021,396:202-214.
APA Guan, Cairu.,Yang, Yong.,Pang, Yaoqi.,Liu, Zebang.,Li, Shenggang.,...&van Bavel, Alexander P..(2021).How CO2 poisons La2O3 in an OCM catalytic reaction: A study by in situ XRD-MS and DFT.JOURNAL OF CATALYSIS,396,202-214.
MLA Guan, Cairu,et al."How CO2 poisons La2O3 in an OCM catalytic reaction: A study by in situ XRD-MS and DFT".JOURNAL OF CATALYSIS 396(2021):202-214.
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