Engineering the low-coordinated single cobalt atom to boost persulfate activation for enhanced organic pollutant oxidation

Engineering the low-coordinated single cobalt atom to boost persulfate activation for enhanced organic pollutant oxidation
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设计低配位单钴原子以促进过硫酸盐活化,从而增强有机污染物氧化

DOI:
10.1016/j.apcatb.2021.120877
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发表时间:
2021-11-23
影响因子:
22.1
通讯作者:
Hu, Chun
Hu, Chun
中科院分区:
化学1区
文献类型:
--
作者:
Liang, Xiaoying;Wang, Di;Hu, Chun

文献摘要

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Two atomically dispersed cobalt catalysts with different nitrogen coordination numbers (denoted as Co-SA-N-x-C) were synthesized and firstly compared to activate peroxydisulfate (PDS) for bisphenol A (BPA) degradation. Theoretical calculations unveiled that lowering the Co-N coordination number from four to three can apparently increase the electron density of the single Co atom in Co-SA-N-3-C to enhance PDS conversion. The low coordinated Co-SA-N-3-C with Co-N-3 coordination structure displays a high specific activity of 0.067 L min(-1) m(-2), which is 1.31 times greater than that of Co-SA-N-4-C with normal Co-N-4 configuration (0.051 L min(-1) m(-2)) in PDS activation. Electron paramagnetic resonance (EPR) measurements and quenching tests confirmed the primary role of sulfate radical (SO4 center dot-) in BPA oxidation over Co-SA-N-3-C with PDS. Moreover, Co-SA-N-3-C delivers favorable durability for PDS activation and potential practicability for realistic wastewater remediation. These findings provide a novel and useful avenue to coordination number modulation of SACs for wider environmental applications.