| 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 Author | Lin, Sen(slin@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn) ; Xie, Zailai(zlxie@fzu.edu.cn) |
| 2020-06-01 | |
| Source Publication | SCIENCE ADVANCES
 |
| ISSN | 2375-2548 |
| Volume | 6Issue:26Pages:9 |
| Abstract | 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. |
| Funding Organization | 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 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Science & Technology - Other Topics |
| WOS Subject | Multidisciplinary Sciences |
| WOS ID | WOS:000543504100027 |
| Publisher | AMER ASSOC ADVANCEMENT SCIENCE |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/139370 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Lin, Sen; Qi, Wei; Xie, Zailai |
| Affiliation | 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 |
| 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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