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

doi:10.1126/sciadv.aba5778

IMR OpenIR

	Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites
	Zhang, Xuefei 1; Yan, Pengqiang 2; Xu, Junkang 1; Li, Fan 2; Herold, Felix 3; Etzold, Bastian J. M.3; Wang, Peng 1; Su, Dang Sheng 2,4; Lin, Sen 1; Qi, Wei 2; Xie, Zailai 1
通讯作者	Lin, Sen(slin@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn) ; Xie, Zailai(zlxie@fzu.edu.cn)
	2020-06-01
发表期刊	SCIENCE ADVANCES
ISSN	2375-2548
卷号	6 期号:26 页码:9
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.
资助者	National Natural Science Foundation of China ; Youth Innovation Promotion Association, Chinese Academy of Sciences ; Deutsche Forschungsgemeinschaft (DFG; German Research Foundation)
DOI	10.1126/sciadv.aba5778
收录类别	SCI
语种	英语
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
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:000543504100027
出版者	AMER ASSOC ADVANCEMENT SCIENCE
引用统计	被引频次：56[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/321006/139373
专题	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.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350016, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromol Chem, D-64287 Darmstadt, Germany 4.Fritz Haber Inst Max Planck Gesell, Faradayweg 4-6, D-14195 Berlin, Germany
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.