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

Xuning Li; Xiang Huang; Shibo Xi; Shu Miao; Jie Ding; Weizheng Cai; Song Liu; Xiaoli Yang; Hongbin Yang; Jiajian Gao; Junhu Wang; Yanqiang Huang; Tao Zhang; Bin Liu

doi:10.1021/jacs.8b05992

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

Xuning Li
, Xiang Huang
, Shibo Xi
, Shu Miao
, Jie Ding
, Weizheng Cai
, Song Liu
, Xiaoli Yang
, Hongbin Yang
, Jiajian Gao
, Junhu Wang
, Yanqiang Huang^*
, Tao Zhang
, Bin Liu

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

1386 Citations (Scopus)

Abstract

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. © 2018 American Chemical Society.

Original language	English
Pages (from-to)	12469-12475
Journal	Journal of the American Chemical Society
Volume	140
Issue number	39
DOIs	https://doi.org/10.1021/jacs.8b05992
Publication status	Published - 3 Oct 2018
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Funding

This work was supported by the National Key Projects for Fundamental Research and Development of China (2016YFA0202804), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17000000), the Dalian Institute of Chemical Physics (DICP DMTO201408), Nanyang Technological University (M4080977.120), the Ministry of Education of Singapore (AcRF Tier 1 M4011021.120 and 2015-T1-002-108), the Agency for Science, Technology and Research (A*Star, M4070178.120 and M4070232.120), and the National Research Foundation (NRF), Prime Minister’s Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program.

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

abstract = "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. {\textcopyright} 2018 American Chemical Society.",

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AU - Li, Xuning

AU - Huang, Xiang

AU - Xi, Shibo

AU - Miao, Shu

AU - Ding, Jie

AU - Cai, Weizheng

AU - Liu, Song

AU - Yang, Xiaoli

AU - Yang, Hongbin

AU - Gao, Jiajian

AU - Wang, Junhu

AU - Huang, Yanqiang

AU - Zhang, Tao

AU - Liu, Bin

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

PY - 2018/10/3

Y1 - 2018/10/3

N2 - 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. © 2018 American Chemical Society.

AB - 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. © 2018 American Chemical Society.

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DO - 10.1021/jacs.8b05992

M3 - RGC 21 - Publication in refereed journal

C2 - 30165734

SN - 0002-7863

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EP - 12475

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

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ER -

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

Abstract

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