Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 40, Pages 21751-21755Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109488
Keywords
degradation; Fe single-atom catalyst; graphitic carbon nitride; organic pollutants; singlet oxygen
Categories
Funding
- National Natural Science Foundation of China [51868050, 52100186, 52170082, 51938007, 51720105001, 51878325]
- Natural Science Foundation of Jiangxi Province [20202BAB213011]
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A novel catalyst Fe-1/CN was developed to achieve 100% selective production of O-1(2) through activation of PMS, enabling highly selective and efficient degradation of organic pollutants.
Singlet oxygen (O-1(2)) is an excellent active species for the selective degradation of organic pollutions. However, it is difficult to achieve high efficiency and selectivity for the generation of O-1(2). In this work, we develop a graphitic carbon nitride supported Fe single-atoms catalyst (Fe-1/CN) containing highly uniform Fe-N-4 active sites with a high Fe loading of 11.2 wt %. The Fe-1/CN achieves generation of 100 % O-1(2) by activating peroxymonosulfate (PMS), which shows an ultrahigh p-chlorophenol degradation efficiency. Density functional theory calculations results demonstrate that in contrast to Co and Ni single-atom sites, the Fe-N-4 sites in Fe-1/CN adsorb the terminal O of PMS, which can facilitate the oxidization of PMS to form SO5.-, and thereafter efficiently generate O-1(2) with 100 % selectivity. In addition, the Fe-1/CN exhibits strong resistance to inorganic ions, natural organic matter, and pH value during the degradation of organic pollutants in the presence of PMS. This work develops a novel catalyst for the 100 % selective production of O-1(2) for highly selective and efficient degradation of pollutants.
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