化学
电子转移
单线态氧
吸附
人体净化
传质
选择性
反应速率常数
膜
蒽
光化学
化学工程
动力学
氧气
催化作用
物理化学
色谱法
有机化学
生物化学
量子力学
物理
工程类
核物理学
作者
Peng Xu,Rui Wei,Peng Wang,Tianyao Shen,Tong Zheng,Guangshan Zhang
标识
DOI:10.1021/acs.est.4c07566
摘要
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), as a promising technology for water decontamination, are constrained by low reaction kinetics due to limited reaction selectivity and mass transfer. Herein, we designed a nanoconfined FeCo2O4-embedded ceramic membrane (FeCo2O4−CM) under flow-through pattern for PMS activation. Confining PMS and FeCo2O4 within nanochannels (3.0−4.7 nm) enhanced adsorption interactions (−7.84 eV vs −2.20 eV), thus boosting mass transfer. Nanoconfinement effect regulated electron transfer pathways from PMS to FeCo2O4−CM by modulating the active site transformation to ≡Co(III) in nanoconfined FeCo2O4−CM, enabling selectively generating 1O2. The primary role of 1O2 in the nanoconfined system was confirmed by kinetic solvent isotope experiments and indicative anthracene endoperoxide (DPAO2). The system enabled 100% removal of atrazine (ATZ) within a hydraulic retention time of 2.124 ms, demonstrating a rate constant over 5 orders of magnitude higher than the nonconfined system (3.50 × 103 s−1 vs 0.42 min−1). It also exhibited strong resilience to pH variations (3.3−9.0) and coexisting substances, demonstrating excellent stability indicated by consistent 100% ATZ removal for 14 days. This study sheds light on regulating electron transfer pathways to selectively generate 1O2 through the nanoconfinement effect, boosting the practical application of PMS-based AOPs in environmental remediation and potentially applying them to various other AOPs.
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