首页|Ca and Sr co-doping induced oxygen vacancies in 3DOM La2-xSrxCe2-yCayO7-δ catalysts for boosting low-temperature oxidative coupling of methane

Ca and Sr co-doping induced oxygen vacancies in 3DOM La2-xSrxCe2-yCayO7-δ catalysts for boosting low-temperature oxidative coupling of methane

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It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macroporous(3DOM)La2-xSrxCe2-yCayO7-δ(A2B2O7-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the acces-sibility of the gaseous reactants(O2 and CH4)to the active sites.The co-doping of Ca and Sr ions in La2-xSrxCe2-yCayO7-δ catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O2-)for the activation of CH4 and the formation of C2 products(C2H6 and C2H4).3DOM La2-xSrxCe2-yCayO7-δ catalysts exhibit high catalytic activity for OCM at low tem-perature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δ catalyst with the highest density of O2-species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4 conversion,selectivity and yield of C2 products at 650 ℃ are 32.2％,66.1％and 21.3％,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.

3DOM catalystsCa ionsSr ionsLow-temperature oxidative coupling of methaneOxygen vacanciesO2- species

Tongtong Wu、Yuechang Wei、Jing Xiong、Yitao Yang、Zhenpeng Wang、Dawei Han、Zhen Zhao、Jian Liu

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State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China

Key Laboratoryof Optical Detection Technology for Oil and Gas,China University of Petroleum,Beijing 102249,China

国家重点研发计划国家重点研发计划国家自然科学基金国家自然科学基金Beijing Nova ProgramScience Foundation of China University of Petroleum,Beijing

2022YFB35041002022YFB35062002220837322376217202204842152462023YJRC030

2024

10.1016/j.jechem.2023.12.025

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.91(4)
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