催化作用
化学
微型反应器
钴
价(化学)
化学工程
矿化(土壤科学)
降级(电信)
光化学
无机化学
有机化学
氮气
工程类
电信
计算机科学
作者
Lin Zhang,Juanjuan Qi,Wenxing Chen,Xiaoyong Yang,Zhimo Fang,Jinmeng Li,Xiuze Li,Siyue Lu,Lidong Wang
标识
DOI:10.1021/acs.est.3c04174
摘要
This study constructed hollow multishelled microreactors with a nanoconfined microenvironment for degrading ofloxacin (OFX) through peroxymonosulfate (PMS) activation in Fenton-like advanced oxidation processes (AOPs), resulting in adequate contaminant mineralization. Among the microreactors, a triple-shelled Co-based hollow microsphere (TS-Co/HM) exhibited optimal performance; its OFX degradation rate was 0.598 min–1, which was higher than that of Co3O4 nanoparticles by 8.97-fold. The structural tuning of Co/HM promoted the formation of oxygen vacancies (VO), which then facilitated the evolution of high-valence cobalt-oxo (Co(IV)═O) and shifted the entire t2g orbital of the Co atom upward, promoting catalytic reactions. Co(IV)═O was identified using a phenylmethyl sulfoxide (PMSO) probe and in situ Raman spectroscopy, and theoretical calculations were conducted to identify the lower energy barrier for Co(IV)═O formation on the defect-rich catalyst. Furthermore, the TS-Co/HM catalyst exhibited remarkable stability in inorganic (Cl–, H2PO4–, and NO3–), organic (humic acid), real water samples (tap water, river water, and hospital water), and in a continuous flow system in a microreactor. The nanoconfined microenvironment could enrich reactants in the catalyst cavities, prolong the residence time of molecules, and increase the utilization efficiency of Co(IV)═O. This work describes an activation process involving Co(IV)═O for organic contaminants elimination. Our results may encourage the use of multishelled structures and inform the design of nanoconfined catalysts in AOPs.
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