Applied Catalysis2022,Vol.30112.DOI:10.1016/j.apcatb.2021.120832

Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process

Lu, Zhijiang Tian, Ziqi Xu, Jianming He, Yan Dou, Jibo Cheng, Jie
Applied Catalysis2022,Vol.30112.DOI:10.1016/j.apcatb.2021.120832

Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process

Lu, Zhijiang 1Tian, Ziqi 2Xu, Jianming 3He, Yan 3Dou, Jibo 3Cheng, Jie3
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作者信息

  • 1. Wayne State Univ, Dept Environm Sci & Geol, Detroit, MI 48201 USA
  • 2. Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Peoples R China
  • 3. Zhejiang Univ, Inst Soil & Water Resources & Environm Sci, Coll Environm & Resource Sci, Hangzhou 310058, Peoples R China
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Abstract

In this study, N/B co-doped biochars were employed as metal-free activators of peroxydisulfate (PDS) for tetracycline degradation, more importantly, the roles of dopants and the relative contribution of radical vs nonradical oxidations were comprehensively investigated. Integrating with electron paramagnetic resonance and kinetics calculations, we showed that co-doping N and B into biochars not only boosted the catalytic activity but also switched the radical PDS-activated process into the electron transfer-dominated nonradical process. Compared with pristine biochar/PDS systems (22%), the nonradical contribution of N/B co-doped biochar/PDS systems increased to 59%, exhibiting outstanding stability and selectivity. Galvanic oxidation tests and theoretical simulations unveiled that doped biochars as conductive tunnels accelerate the potential difference-driven electron transfer from the highest occupied molecular orbital of pollutants to the lowest unoccupied molecular orbital of PDS due to the lower energy gap. This study provided new insights into the critical role of heteroatom-doped carbocatalysts in PDS nonradical activation.

Key words

Biochar/Heteroatoms doping/Peroxydisulfate activation/Electron transfer/Theoretical calculations

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN:0926-3373
被引量110
参考文献量63
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