title: The optimization, kinetics and mechanism of m-cresol degradation via catalytic wet peroxide oxidation with sludge-derived carbon catalyst.
abstract: The sludge-derived carbon catalyst modified with 0°C HNO3solution was tested in catalytic wet peroxide oxidation of m-cresol (100mgL-1) with systematical mathematical models and theoretical calculation for the first time. The reaction conditions were optimized by response surface methodology (RSM) as T=60°C, initial pH=3.0, C0,H2O2(30%)=1.20gL-1(lower than the stoichiometric amount of 1.80gL-1) and Ccat=0.80gL-1, with 96% of m-cresol and 47% of TOC converted after 16min and 120min of reaction, respectively, and ξ (mg TOC/g H2O2fed)=83.6mg/g. The end time of the first kinetic period in m-cresol model was disclosed to be correlated with the fixed residue m-cresol concentration of about 33%. Furthermore, the kinetic constants in models of TOC and H2O2exactly provide convincing proof of three-dimensional response surfaces analysis by RSM, which showed the influence of the interaction between organics and H2O2on effective H2O2utilization. The reaction intermediates over time were identified by gas chromatography-mass spectrometer based on kinetics analysis. Four degradation pathways for m-cresol were proposed, of which the possibility and feasibility were well proven by frontier molecule orbital theory and atomic charge distribution via density functional theory method.
authors.affiliation: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.
authors.forename: Yamin
authors.initials: Y
authors.lastname: Wang
authors.affiliation: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China.
authors.forename: Huangzhao
authors.initials: H
authors.lastname: Wei
authors.affiliation: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China.
authors.forename: Ying
authors.initials: Y
authors.lastname: Zhao
authors.affiliation: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.
authors.forename: Wenjing
authors.initials: W
authors.lastname: Sun
authors.affiliation: Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, PR China. Electronic address: clsun@dicp.ac.cn.
authors.forename: Chenglin
authors.initials: C
authors.lastname: Sun
keywords: Catalytic wet peroxide oxidation; Density functional theory; Kinetics; Response surface methodology; Sludge-derived carbon catalyst