Bromine-mediated conversion of methane to C1 oxygenates over Zn-MCM-41 supported mercuric oxide

doi:10.1016/j.apcata.2007.11.014

CORC > 化学研究所 > 中国科学院化学研究所

	Bromine-mediated conversion of methane to C1 oxygenates over Zn-MCM-41 supported mercuric oxide
	Li, Fengbo; Yuan, Guoqing; Yan, Fang; Yan, Fengwen
刊名	APPLIED CATALYSIS A-GENERAL
	2008-02-01
卷号	335 期号:1 页码:82-87
关键词	Bromine Methane Selective Oxidation C1 Oxygenates Mercuric Oxide
ISSN号	0926-860X
DOI	10.1016/j.apcata.2007.11.014
英文摘要	The structure mobility of the zigzag mercuric oxide chains and the strong preference of mercuric (11) cation sites for bromine lead to a novel bromine-mediated partial methane oxidation at relatively low reaction temperature (220 degrees C). Zn-MCM-41 supported mercuric oxide nanophases were used as the model catalyst to investigate the role of bromine in the catalytic cycle. The introduction of bromine to feed gas consisting of CH4/O-2/Ar (3:1:6) leads to a sharp increase in the methane conversion. Meanwhile, a transient high product selectivity to C 1 oxygenates was observed. Two bromine-mediated routes can be identified: MeHgBrn as the intermediate species and mercuric hypobromite as the active agent for methane oxidation, which occur simultaneously in the methane conversion. The controlling mechanism transfers from the former to the latter with the gradual fixation of bromine into mercuric oxide lattice. The catalyst was characterized detailedly by XRD, XPS, and N-2 Sorption. The chemical composite changes of active species were detected by XPS, which provide some direct information about the mediator role of bromine in the catalytic cycle. (C) 2007 Elsevier B.V. All rights reserved.
语种	英语
出版者	ELSEVIER SCIENCE BV
WOS记录号	WOS:000253366100011
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/63869]
专题	中国科学院化学研究所
通讯作者	Yuan, Guoqing
作者单位	Chinese Acad Sci, BNLMS, Inst Chem, Lab New Mat, Beijing 100080, Peoples R China
推荐引用方式 GB/T 7714	Li, Fengbo,Yuan, Guoqing,Yan, Fang,et al. Bromine-mediated conversion of methane to C1 oxygenates over Zn-MCM-41 supported mercuric oxide[J]. APPLIED CATALYSIS A-GENERAL,2008,335(1):82-87.
APA	Li, Fengbo,Yuan, Guoqing,Yan, Fang,&Yan, Fengwen.(2008).Bromine-mediated conversion of methane to C1 oxygenates over Zn-MCM-41 supported mercuric oxide.APPLIED CATALYSIS A-GENERAL,335(1),82-87.
MLA	Li, Fengbo,et al."Bromine-mediated conversion of methane to C1 oxygenates over Zn-MCM-41 supported mercuric oxide".APPLIED CATALYSIS A-GENERAL 335.1(2008):82-87.