Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis

Li, Xuning1,3; Huang, Xiang4; Xi, Shibo5; Miao, Shu1; Ding, Jie1; Cai, Weizheng3; Liu, Song1,3,6; Yang, Xiaoli1,6; Yang, Hongbin3; Gao, Jiajian3; Wang, Junhu1,2; Huang, Yanqiang1; Zhang, Tao1,6; Liu, Bin3

2018-10-03

10.1021/jacs.8b05992

Journal of the American Chemical Society   影响因子和分区

0002-7863

The Fenton-like process presents one of the most promising strategies to generate reactive oxygen-containing radicals to deal with the ever-growing environmental pollution. However, developing improved catalysts with adequate activity and stability is still a long-term goal for practical application. Herein, we demonstrate single cobalt atoms anchored on porous N-doped graphene with dual reaction sites as highly reactive and stable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). Our experiments and density functional theory (DFT) calculations show that the CoN4 site with a single Co atom serves as the active site with optimal binding energy for PMS activation, while the adjacent pyrrolic N site adsorbs organic molecules. The dual reaction sites greatly reduce the migration distance of the active singlet oxygen produced from PMS activation and thus improve the Fenton-like catalytic performance.

SCI ; EI

英语

NI期刊 ; NI论文 ; ESI高被引

其他

Agency for Science, Technology and Research (A*Star)[M4070178.120]

Chemistry

Chemistry, Multidisciplinary

WOS:000446920100028

AMER CHEMICAL SOC

20183805826651

Activation energy ; Atoms ; Binding energy ; Catalyst activity ; Catalytic oxidation ; Cobalt ; Density functional theory ; Doping (additives) ; Graphene ; Oxygen

Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

Web of Science

1.Chinese Acad Sci, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Mossbauer Effect Data Ctr, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore
4.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
5.ASTAR, Inst Chem & Engn Sci, 1 Pesek Rd, Singapore 627833, Singapore
6.Univ Chinese Acad Sci, Beijing 100049, Peoples R China

Li, Xuning,Huang, Xiang,Xi, Shibo,et al. Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis[J]. Journal of the American Chemical Society,2018,140(39):12469-12475.

Li, Xuning.,Huang, Xiang.,Xi, Shibo.,Miao, Shu.,Ding, Jie.,...&Liu, Bin.(2018).Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis.Journal of the American Chemical Society,140(39),12469-12475.

Li, Xuning,et al."Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis".Journal of the American Chemical Society 140.39(2018):12469-12475.