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Methanol conversion on borocarbonitride catalysts: Identification and quantification of active sites
Zhang, Xuefei1; Yan, Pengqiang2; Xu, Junkang1; Li, Fan2; Herold, Felix3; Etzold, Bastian J. M.3; Wang, Peng1; Su, Dang Sheng2,4; Lin, Sen1; Qi, Wei2; Xie, Zailai1
Corresponding AuthorLin, Sen(slin@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn) ; Xie, Zailai(zlxie@fzu.edu.cn)
2020-06-01
Source PublicationSCIENCE ADVANCES
ISSN2375-2548
Volume6Issue:26Pages:9
AbstractBorocarbonitrides (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.
Funding OrganizationNational Natural Science Foundation of China ; Youth Innovation Promotion Association, Chinese Academy of Sciences ; Deutsche Forschungsgemeinschaft (DFG; German Research Foundation)
DOI10.1126/sciadv.aba5778
Indexed BySCI
Language英语
Funding ProjectNational 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 Research AreaScience & Technology - Other Topics
WOS SubjectMultidisciplinary Sciences
WOS IDWOS:000543504100027
PublisherAMER ASSOC ADVANCEMENT SCIENCE
Citation statistics
Cited Times:5[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/139373
Collection中国科学院金属研究所
Corresponding AuthorLin, Sen; Qi, Wei; Xie, Zailai
Affiliation1.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
Recommended Citation
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.
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