Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites

doi:10.1126/sciadv.aba5778

CORC > 金属研究所 > 中国科学院金属研究所

	Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites
	Zhang, Xuefei 4; Yan, Pengqiang 2; Xu, Junkang 4; Li, Fan 2; Herold, Felix 1; Etzold, Bastian J. M.1; Wang, Peng 4; Su, Dang Sheng 2,3; Lin, Sen 4; Qi, Wei 2
刊名	SCIENCE ADVANCES
	2020-06-01
卷号	6 期号:26 页码:9
ISSN号	2375-2548
DOI	10.1126/sciadv.aba5778
通讯作者	Lin, Sen(slin@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn) ; Xie, Zailai(zlxie@fzu.edu.cn)
英文摘要	Borocarbonitrides (BCNs) have emerged as highly selective catalysts for the oxidative dehydrogenation (ODH) reaction. However, there is a lack of in-depth understanding of the catalytic mechanism over BCN catalysts due to the complexity of the surface oxygen functional groups. Here, BCN nanotubes with multiple active sites are synthesized for oxygen-assisted methanol conversion reaction. The catalyst shows a notable activity improvement for methanol conversion (29%) with excellent selectivity to formaldehyde (54%). Kinetic measurements indicate that carboxylic acid groups on BCN are responsible for the formation of dimethyl ether, while the redox catalysis to formaldehyde occurs on both ketonic carbonyl and boron hydroxyl (B-OH) sites. The ODH reaction pathway on the B-OH site is further revealed by in situ infrared, x-ray absorption spectra, and density functional theory. The present work provides physical-chemical insights into the functional mechanism of BCN catalysts, paving the way for further development of the underexplored nonmetallic catalytic systems.
资助项目	National Natural Science Foundation of China[21761132010] ; National Natural Science Foundation of China[91645114] ; National Natural Science Foundation of China[21573256] ; National Natural Science Foundation of China[21571035] ; National Natural Science Foundation of China[21673040] ; National Natural Science Foundation of China[51521091] ; Youth Innovation Promotion Association, Chinese Academy of Sciences ; Deutsche Forschungsgemeinschaft (DFG; German Research Foundation)[ET-101/13-1]
WOS研究方向	Science & Technology - Other Topics
语种	英语
出版者	AMER ASSOC ADVANCEMENT SCIENCE
WOS记录号	WOS:000543504100027
资助机构	National Natural Science Foundation of China ; Youth Innovation Promotion Association, Chinese Academy of Sciences ; Deutsche Forschungsgemeinschaft (DFG; German Research Foundation)
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/139369]
专题	金属研究所_中国科学院金属研究所
通讯作者	Lin, Sen; Qi, Wei; Xie, Zailai
作者单位	1.Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromol Chem, D-64287 Darmstadt, Germany 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Fritz Haber Inst Max Planck Gesell, Faradayweg 4-6, D-14195 Berlin, Germany 4.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350016, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Xuefei,Yan, Pengqiang,Xu, Junkang,et al. Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites[J]. SCIENCE ADVANCES,2020,6(26):9.
APA	Zhang, Xuefei.,Yan, Pengqiang.,Xu, Junkang.,Li, Fan.,Herold, Felix.,...&Xie, Zailai.(2020).Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites.SCIENCE ADVANCES,6(26),9.
MLA	Zhang, Xuefei,et al."Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites".SCIENCE ADVANCES 6.26(2020):9.