Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 39, Pages 12469-12475Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b05992
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Funding
- National Key Projects for Fundamental Research and Development of China [2016YFA0202804]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Dalian Institute of Chemical Physics [DICP DMTO201408]
- Nanyang Technological University [M4080977.120]
- Ministry of Education of Singapore (AcRF Tier 1) [M4011021.120, 2015-T1-002-108]
- Agency for Science, Technology and Research (A*Star) [M4070178.120, M4070232.120]
- National Research Foundation (NRF), Prime Minister's Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program
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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.
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