Direct Conversion of Methane to Value-Added Chemicals over Heterogeneous Catalysts: Challenges and Prospects

被引:1039
|
作者
Schwach, Pierre [1 ]
Pan, Xiulian [1 ]
Bao, Xinhe [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[2] Fudan Univ, Chem Dept, Shanghai 200433, Peoples R China
基金
中国国家自然科学基金;
关键词
DENSITY-FUNCTIONAL THEORY; HYDROGEN-ATOM TRANSFER; THERMAL UNIMOLECULAR REACTIONS; RADIAL CONCENTRATION GRADIENTS; LOADED FEOX/SIO2 CATALYSTS; REACTOR MODELING-CRITERIA; MAGNESIUM-OXIDE CATALYST; COLLISION RATE CONSTANTS; PERIODIC CH4-H-2 SWITCH; MO-95; NMR-SPECTROSCOPY;
D O I
10.1021/acs.chemrev.6b00715
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The quest for an efficient process to convert methane efficiently to fuels and high value-added chemicals such as olefins and aromatics is motivated by their increasing demands and recently discovered large reserves and resources of methane. Direct conversion to these chemicals can be realized either oxidatively via oxidative coupling of methane (OCM) or nonoxidatively via methane dehydroaromatization (MDA), which have been under intensive investigation for decades. While industrial applications are still limited by their low yield (selectivity) and stability issues, innovations in new catalysts and concepts are needed. The newly emerging strategy using iron single sites to catalyze methane conversion to olefins, aromatics, and hydrogen (MTOAH) attracted much attention when it was reported. Because the challenge lies in controlled dehydrogenation of the highly stable CH4 and selective C-C coupling, we focus mainly on the fundamentals of C-H activation and analyze the reaction pathways toward selective routes of OCM, MDA, and MTOAH. With this, we intend to provide some insights into their reaction mechanisms and implications for future development of highly selective catalysts for direct conversion of methane to high value-added chemicals.
引用
收藏
页码:8497 / 8520
页数:24
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