Applied Catalysis2022，Vol.31212.DOI:10.1016/j.apcatb.2022.121408

Tailoring the coordination environment of cobalt in a single-atom catalyst through phosphorus doping for enhanced activation of peroxymonosulfate and thus efficient degradation of sulfadiazine

Zou, Yubin Hu, Jiahui Li, Bing Lin, Lin Li, Yin Liu, Feifei Li, Xiao-yan
Applied Catalysis2022，Vol.31212.DOI:10.1016/j.apcatb.2022.121408
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  • NSTL
  • Elsevier

Tailoring the coordination environment of cobalt in a single-atom catalyst through phosphorus doping for enhanced activation of peroxymonosulfate and thus efficient degradation of sulfadiazine

Zou, Yubin 1Hu, Jiahui 1Li, Bing 1Lin, Lin 1Li, Yin 1Liu, Feifei 1Li, Xiao-yan1
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作者信息

  • 1. Tsinghua Univ
  • 折叠

Abstract

The catalytic activity of single-atom catalysts (SACs) can be enhanced by engineering the coordination environment of metal centres. Herein, zeolitic imidazolate framework (ZIF) was used as a precursor to introduce P atoms into a Co-based SAC. With the P doping, the resultant ZIF-CoN3P-C could efficiently degrade 98.4% of sulfadiazine (10 mg L-1) within 5 min by activating peroxymonosulfate (PMS) with an elevated degradation rate constant 2.5 times that of ZIF-CoN4-C. Density functional theory (DFT) calculations indicate that the electron density and electron delocalisation were further concentrated around the Co centres by the P doping, which facilitated electron transfer from Co to PMS molecules and enhanced the generation of singlet oxygen (O-1(2)). The ZIF-CoN4P-C exhibited its universality and stability for the PMS-based oxidation process. Overall, these findings clarify the role of P atoms in tuning the electronic structure and reactivity of Co in ZIF-CoN3P-C for enhanced PMS activation and organic degradation.

Key words

PMS activation/Single-atom catalysts/Coordination environment/Organic degradation/Cobalt catalysts/METAL-ORGANIC FRAMEWORKS/HETEROGENEOUS CATALYSIS/FENTON OXIDATION/OXYGEN/ELECTROCATALYSTS/GENERATION/INSIGHTS/WATER

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN：0926-3373
被引量58
参考文献量69
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