| Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C | |
| Huang, Kuntao1; Fu, Hongquan1; Shi, Wen2; Wang, Hongjuan1; Cao, Yonghai1; Yang, Guangxing1; Peng, Feng3; Wang, Qiang4; Liu, Zhigang5; Zhang, Bingsen2; Yu, Hao1 | |
| Corresponding Author | Zhang, Bingsen(bszhang@imr.ac.cn) ; Yu, Hao(yuhao@scut.edu.cn) |
| 2019-09-01 | |
| Source Publication | JOURNAL OF CATALYSIS
 |
| ISSN | 0021-9517 |
| Volume | 377Pages:283-292 |
| Abstract | Me-N-C catalysts have received intensive scientific interest as non-noble-metal single-atom catalysts (SAC) for electrochemical- and thermocatalytic reactions. However, the lack of understanding of its properties hinders further improvement of the catalytic performance. An interesting issue is the molecular details of the reaction involving more than one reactant, since the activation of the second reactant is inevitably affected by the first one on SAC. Here, we synthesized Co-N-C SACs for the aerobic oxidation of benzyl alcohol (BA) to benzaldehyde. The catalyst exhibited excellent activity for this reaction, among the most active non-noble-metal catalysts. Differently from particulate metal or metal oxide catalysts, the Co-N-C SAC displayed "self-poisoning" due to the strong competitive adsorption of BA to O-2, as revealed by kinetics experiments and density functional theory calculations. Moreover, we rationalized the poisoning effect of polar moieties, including organic solvents and aqueous solutions, on the SAC. These results shed light on the catalytic behavior of aerobic oxidation of BA on the molecular level and enable the rational design of catalytic organic synthesis over Co-N-C SACs. (C) 2019 Elsevier Inc. All rights reserved. |
| Keyword | Co-N-C Single-atom catalyst Benzyl alcohol oxidation Kinetics DFT calculation |
| Funding Organization | National Natural Science Foundation of China (NSFC) ; Guangdong Natural Science Foundation ; Science and Technology Program of Guangzhou City ; NSFC ; Youth INnuovation Promotion Association CAS |
| DOI | 10.1016/j.jcat.2019.06.047 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | National Natural Science Foundation of China (NSFC)[21676100] ; National Natural Science Foundation of China (NSFC)[21872041] ; Guangdong Natural Science Foundation[2017A030312005] ; Science and Technology Program of Guangzhou City[201707010058] ; NSFC[21773269] ; Youth INnuovation Promotion Association CAS[20151521] |
| WOS Research Area | Chemistry ; Engineering |
| WOS Subject | Chemistry, Physical ; Engineering, Chemical |
| WOS ID | WOS:000491683200028 |
| Publisher | ACADEMIC PRESS INC ELSEVIER SCIENCE |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/136991 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Zhang, Bingsen; Yu, Hao |
| Affiliation | 1.South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 3.Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Guangdong, Peoples R China 4.Nanjing Tech Univ, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Inst Adv Synth, Sch Chem & Mol Engn, Nanjing 211816, Jiangsu, Peoples R China 5.Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China |
| Recommended Citation GB/T 7714 | Huang, Kuntao,Fu, Hongquan,Shi, Wen,et al. Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C[J]. JOURNAL OF CATALYSIS,2019,377:283-292. |
| APA | Huang, Kuntao.,Fu, Hongquan.,Shi, Wen.,Wang, Hongjuan.,Cao, Yonghai.,...&Yu, Hao.(2019).Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C.JOURNAL OF CATALYSIS,377,283-292. |
| MLA | Huang, Kuntao,et al."Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C".JOURNAL OF CATALYSIS 377(2019):283-292. |
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