The iron-based biochar activating chlorite(ClO_(2)^(−))driven by mechanochemical ultrasonic:piecewise kinetics,biomimetic catalytic-mechanism,and novel advanced redox process  

作　　者：Qihui Xu Qianhui Yang Yuming Xie Lin Hu Zhenghao Fei Hong You 

机构地区：[1]School of Chemical and Environmental Engineering,Yancheng Teachers University,Yancheng 224007,China [2]State Key Laboratory of Urban Water Resources and Environment,Harbin Institute of Technology,Harbin 150090,China [3]School of Marine Science and Technology,Harbin Institute of Technology at Weihai,Weihai 264209,China

出　　处：《Frontiers of Environmental Science & Engineering》2025年第2期151-168,共18页环境科学与工程前沿(英文)

基　　金：supported by the Natural Science foundation of the Jiangsu Higher Education Institutions(No.24KJB610019);the Scientific Research Foundation of Yancheng Teachers University(No.204060047);the Horizontal Topic Research“Developing the environmental remediation technology by acoustic catalysis”(No.203060199).

摘　　要：Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utilized to activate COI(2 mmol/L)to present selective oxidation in removing triphenylmethane derivatives(15 min,90%).The protonation(H+at~102μmol/L level)played a huge role(k-2nd=0.136c-H+−0.014(R^(2)-adj=0.986),and rapp=−0.0876/c-H++1.017(R^(2)-adj=0.996))to boost the generation of the active species(e.g.,high-valent iron oxidizing species(HVI=O)and chlorine dioxide(ClO_(2))).The protonation-coupled electron transfer promoted Fe-substances in Feb/HCs activating COI(the calculated kobs ranging from 0.066−0.285 min^(−1)).The form of ClO_(2) mainly attributed to proton-coupled electron transfer(1e/1H+).The HVI=O was generated from the electron transfer within the coordination complex.Moreover,carbon particles in FebHCs serve as the bridge for electron transfer.The above roles contribute to the fracture and formation of coordination-induced bonds between Lx-FeII/III and ClO_(2)^(−)at phase interface to form AROP.The ultrasonic(US)cavitation enhanced the mass transfer of active species in bulk solution,and the HVI=O and ClO_(2) attack unsaturated central carbon atoms of triphenylmethane derivatives to initiate selective removal.Furthermore,the scale-up experiment with continuous flow(k values of approximately 0.2 min^(−1),COD removal efficiency of approximately 80%)and the reactor with COMSOL simulation have also proved the applicability of the system.The study offers a novel AROP and new insights into correspondingly heterogeneous interface activation mechanisms.

关 键 词：CHLORITE Iron-based biochar ULTRASONIC Chlorine dioxide High-valent iron oxidizing species 

分 类 号：O62[理学—有机化学]