期刊
ADVANCED FUNCTIONAL MATERIALS
卷 31, 期 13, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202007877
关键词
carbon nitride; Fenton-like reaction; molecular engineering; photocatalysis; single-atom catalysis
类别
资金
- Zhejiang Province Basic Public Welfare Research Project [LGF19B070006]
- National Natural Science Foundation of China [21775138]
- Hangzhou Municipal Health Commission
- Hangzhou Science and Technology Bureau [A20200043]
- Pawsey Supercomputing Centre
A novel transition metal single-atom catalyst has been developed for efficient heterogeneous Fenton-like reactions, showing excellent cyclic stability and a wide effective pH range. The catalyst accelerates the production and separation of charge carriers, enhancing the reaction performance.
Heterogeneous Fenton-like reactions (HFLR) are promising alternative strategies to address the inherent limitations of the classic Fenton systems. Herein, a facile and scale-up approach for the synthesis of transition metal single-atom sites (SA-TM, TM = Cr, Mn, Fe, Co, Cu) coordinated onto pyrrolic N-rich g-C3N4 (PN-g-C3N4) scaffold is developed. The regulated pyrrolic N-rich SA-TM catalytic sites exhibit excellent performances for HFLR. As a model of SA-TM/PN-g-C3N4, SA-Cr/PN-g-C3N4 is efficient for the catalytic oxidation of bisphenol A via HFLR under visible light with outstanding cyclic stability and wide effective pH range (3.0-11.0). The synergy of photocatalysis and single-atom catalysis leads to accelerated production and separation of charge carriers as well as the cycling of Cr3+/Cr2+ couple, consequently boosting the performance in HFLR. Theoretical calculations indicate that the Cr(II)-N-4 sites with the metalloporphyrin-like structure are more reactive than the doped Cr(II) sites in the g-C3N4 matrix, which act as the peroxidase-mimicking nanozyme for efficient and homolytic cleavage of peroxide O-O in H2O2. This study expands the family of the iron-free Fenton-like systems and provides new strategies to the rational design and precise regulation of on-demand multifunctional single-atom catalysts for advanced water remediation.
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