N,O-Codoped Onion-like Carbon Catalyzed Selective Oxidation of Methanol to Dimethoxymethane: Structure-Activity Relationship

doi:10.1002/cctc.202300813

IMR OpenIR

	N,O-Codoped Onion-like Carbon Catalyzed Selective Oxidation of Methanol to Dimethoxymethane: Structure-Activity Relationship
	Bai, Yunli L.1,2; Dai, Xueya 1,2; Cao, Tianlong L.2; Qi, Wei 1,2
通讯作者	Dai, Xueya(xydai19b@imr.ac.cn) ; Qi, Wei(wqi@imr.ac.cn)
	2023-11-23
发表期刊	CHEMCATCHEM
ISSN	1867-3880
页码	9
摘要	One-step synthesis of dimethoxymethane (DMM) via methanol oxidation under the catalysis of nanocarbon is a green and sustainable chemical industrial process. In this work, nitrogen, oxygen codoped onion-like carbon (NOLC) were prepared via a simple thermal treatment method, which was applied to one-step synthesis of DMM. The physicochemical characterization results revealed that nitrogen and oxygen elements were successfully introduced into the onion-like carbon (OLC) catalyst. The proposed NOLC catalysts exhibited DMM selectivity of 75 % at relatively low reaction temperature (150 degrees C) and long stability over 10 h. In-situ titration experiments revealed that the carboxylic acid groups on NOLC surface were the main acidic active sites. The Clemmensen reduction control experiment revealed that the carbonyl groups were the active sites for the formation of formaldehyde. The basic reaction kinetics and mechanism such as reaction orders, apparent activation energy and rate determining step etc. for one-step synthesis of DMM via methanol were studied systematically. The present work shows an important structure-function relation for designing highly efficient nanocarbon catalyzed methanol conversion reaction system that the appropriate redox/acid intensity on catalyst surface through the modulation of N and O elements would effectively improve the selectivity of DMM. Nitrogen, oxygen codoped onion-like carbon exhibits relatively high dimethoxymethane (DMM) selectivity from methanol at low reaction temperature (150 degrees C). The present research does not only demonstrate that nanocarbon is a promising catalyst for one-step synthesis of DMM but also highlights the key to increase the selectivity of DMM is to balance the redox and acidity of carbon catalysts.image
关键词	methanol oxidation dehydrogenation nanocarbon materials nitrogen-oxygen co-doped onion-like carbon one-step synthesis selectivity of DMM
资助者	NSFC of China ; Natural Science Foundation of Liaoning Province of China
DOI	10.1002/cctc.202300813
收录类别	SCI
语种	英语
资助项目	NSFC of China ; Natural Science Foundation of Liaoning Province of China[2020-YQ-02] ; [22072163]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:001106924000001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：2[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/177292
专题	中国科学院金属研究所
通讯作者	Dai, Xueya; Qi, Wei
作者单位	1.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Bai, Yunli L.,Dai, Xueya,Cao, Tianlong L.,et al. N,O-Codoped Onion-like Carbon Catalyzed Selective Oxidation of Methanol to Dimethoxymethane: Structure-Activity Relationship[J]. CHEMCATCHEM,2023:9.
APA	Bai, Yunli L.,Dai, Xueya,Cao, Tianlong L.,&Qi, Wei.(2023).N,O-Codoped Onion-like Carbon Catalyzed Selective Oxidation of Methanol to Dimethoxymethane: Structure-Activity Relationship.CHEMCATCHEM,9.
MLA	Bai, Yunli L.,et al."N,O-Codoped Onion-like Carbon Catalyzed Selective Oxidation of Methanol to Dimethoxymethane: Structure-Activity Relationship".CHEMCATCHEM (2023):9.