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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]) |
ISSN | 0021-9517 |
EISSN | 1090-2694 |
卷号 | 396页码:202-214 |
发表状态 | 已发表 |
DOI | 10.1016/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 |
引用统计 | 正在获取...
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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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