Insight into the Formation of Co@Co2C Catalysts for Direct Synthesis of Higher Alcohols and Olefins from Syngas

doi:10.1021/acscatal.7b02403

	Insight into the Formation of Co@Co2C Catalysts for Direct Synthesis of Higher Alcohols and Olefins from Syngas
	Zhao, Ziang 1,2; Lu, Wei 1; Yang, Ruoou 2,4; Zhu, Hejun 1; Dong, Wenda 1; Sun, Fanfei 2,4; Jiang, Zheng 4; Lyu, Yuan 1; Liu, Tao 1; Du, Hong 1
刊名	ACS CATALYSIS
	2018
卷号	8 期号:1 页码:228-241
关键词	Higher Alcohols Olefins Fischer-tropsch Synthesis Mn Promoter Cobalt Carbide
ISSN号	2155-5435
DOI	10.1021/acscatal.7b02403
文献子类	Article
英文摘要	Cobalt carbide (Co2C) has recently been reported to be efficient for the conversion of syngas (CO+H-2) to lower olefins (C-2-C-4) and higher alcohols (C2+, alcohols); however, its properties and formation conditions remain ambiguous. On the basis of our previous investigations concerning the formation of Co2C, the work herein was aimed at defining the mechanism by which the manganese promoter functions in the Co-based catalysts supported on activated carbon (CoxMn/AC). Experimental studies validated that Mn facilitates the dissociation and disproportionation of CO on the surface of catalyst and prohibits H-2 adsorption to some extent, creating a relative C-rich and H-lean surface chemical environment. We advocate that the surface conditions result in the transformation from metallic Co to Co2C phase under realistic reaction conditions to form Co@Co2C nanoparticles, in which residual small Co-0 ensembles (<6 nm) distribute on the surface of Co2C nanoparticles (similar to 20 nm). Compared with the Co/AC catalyst, where the active site is composed of Co2C phase on the surface of Co-0 nanoparticles (Co2C@Co), the Mn-promoted catalysts (Co@Co2C) displayed much higher olefin selectivity (10% versus 40%), while the selectivity to alcohols over the two catalysts are similar (similar to 20%). The rationale behind the strong structure performance relationship is twofold. On the one hand, Co Co2C interfaces exist universally in the catalysts, where synergistic effects between metallic Co and Co2C phase occur and are responsible for the formation of alcohols. On the other hand, the relative C-rich environment created by Mn on the Co@Co2C catalysts facilitates the formation of olefins.
WOS关键词	FISCHER-TROPSCH SYNTHESIS ; SUPPORTED COBALT CATALYSTS ; PROMOTED CO/AC CATALYSTS ; CO HYDROGENATION ; MANGANESE OXIDE ; LIGHT OLEFINS ; MN PROMOTION ; SELECTIVITY ; CARBON ; CARBIDE
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000419751100026
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/168480]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Zhu, Hejun; Jiang, Zheng; Ding, Yunjie
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
推荐引用方式 GB/T 7714	Zhao, Ziang,Lu, Wei,Yang, Ruoou,et al. Insight into the Formation of Co@Co2C Catalysts for Direct Synthesis of Higher Alcohols and Olefins from Syngas[J]. ACS CATALYSIS,2018,8(1):228-241.
APA	Zhao, Ziang.,Lu, Wei.,Yang, Ruoou.,Zhu, Hejun.,Dong, Wenda.,...&Ding, Yunjie.(2018).Insight into the Formation of Co@Co2C Catalysts for Direct Synthesis of Higher Alcohols and Olefins from Syngas.ACS CATALYSIS,8(1),228-241.
MLA	Zhao, Ziang,et al."Insight into the Formation of Co@Co2C Catalysts for Direct Synthesis of Higher Alcohols and Olefins from Syngas".ACS CATALYSIS 8.1(2018):228-241.