Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C

doi:10.1016/j.jcat.2019.06.047

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	Competitive adsorption on single-atom catalysts: Mechanistic insights into the aerobic oxidation of alcohols over Co-N-C
	Huang, Kuntao 1; Fu, Hongquan 1; Shi, Wen 2; Wang, Hongjuan 1; Cao, Yonghai 1; Yang, Guangxing 1; Peng, Feng 3; Wang, Qiang 4; Liu, Zhigang 5; Zhang, Bingsen 2
刊名	JOURNAL OF CATALYSIS
	2019-09-01
卷号	377 页码:283-292
关键词	Co-N-C Single-atom catalyst Benzyl alcohol oxidation Kinetics DFT calculation
ISSN号	0021-9517
DOI	10.1016/j.jcat.2019.06.047
通讯作者	Zhang, Bingsen(bszhang@imr.ac.cn) ; Yu, Hao(yuhao@scut.edu.cn)
英文摘要	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.
资助项目	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研究方向	Chemistry ; Engineering
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000491683200028
资助机构	National Natural Science Foundation of China (NSFC) ; Guangdong Natural Science Foundation ; Science and Technology Program of Guangzhou City ; NSFC ; Youth INnuovation Promotion Association CAS
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/136990]
专题	金属研究所_中国科学院金属研究所
通讯作者	Zhang, Bingsen; Yu, Hao
作者单位	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
推荐引用方式 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.