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

被引：90
作者：
Liang, Xiaoying [1 ]
Wang, Di [1 ]
Zhao, Zhiyu [1 ]
Li, Tong [1 ]
Chen, Zhenhuan [1 ]
Gao, Yaowen [1 ]
Hu, Chun [1 ]
机构：
[1] Guangzhou Univ, Inst Environm Res Greater Bay, Key Lab Water Qual & Conservat Pearl River Delta, Minist Educ, Guangzhou 510006, Peoples R China
来源：
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 303卷
基金：
中国国家自然科学基金;
关键词：
Single-atom catalysts; Coordination number; Electron density; Persulfate conversion; Active radicals; WATER-TREATMENT; DEGRADATION; PEROXYMONOSULFATE; CARBON; CONTAMINANTS; CHALLENGES; GENERATION; FRAMEWORKS; CATALYSIS; RADICALS;
D O I：
10.1016/j.apcatb.2021.120877
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
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.
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页数：11
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