Conversion of carbonaceous materials into solid acids for tylosin mitigation:effect of preprocessing methods on the reactivity of sulfonation reaction  

作　　者：Chunmei Wang Qianqian Xie Xiaomin Dou Lanxi Zhang Xiao Yang 

机构地区：[1]College of Environmental Science and Engineering,Beijing Forestry University,Beijing 100083,People’s Republic of China [2]Key Laboratory of Land Surface Pattern and Simulation,Institute of Geographic Sciences and Natural Resources Research,Chinese Academy of Sciences,Beijing 100101,People’s Republic of China

出　　处：《Biochar》2023年第1期558-573,共16页生物炭（英文）

基　　金：National Natural Science Foundation of China(51978052,42207456);State Key Joint Laboratory of Environmental Simulation and Pollution(19K01ESPCR).

摘　　要：Carbon-based solid acids have been successfully employed as acidic catalysts for pollutant mitigation in wastewater.To fully tap the potentials of commercially viable carbons for the preparation of solid acids and enhance their catalytic performances is a challenging problem.In this work,three commercialized carbons including biochar,activated carbon and graphite were preprocessed(ball-milling,Hummer exfoliation,HNO3 soaking,and microwave heating in HNO_(3),etc.),sulfonated,and evaluated as solid-acid catalysts for tylosin mitigation.Graphite-originated solid acid performed the best through a balling-milling preprocess,while biochar-originated solid acids behaved well under all preprocessing treatments,in which 40 mg L^(−1) of tylosin was mitigated within 8 min by 1 g L^(−1) of biochar-originated solid acids.The biochar solid acid through the ball-milling preprocess presented high total acidity and large amounts of-SO_(3)H groups,due to dramatically increased surface area and the rise of activation groups(hydroxyl,alkyl and alkoxy groups,etc.)facilitating electrophilic reaction.In addition,decreased particle size and aromaticity and increased structural defects also contributed.Theoretical calculation of average local ionization energy(ALIE)of condensed aromatic model molecules with substituted activation groups confirmed the promoting effects on sulfonation from strong to weak were 8.40-9.06 eV.These findings have deepened the knowledge in tuning carbon surface chemistry for better sulfonation,thus strengthening catalytic degradation of tylosin.The value of this study is in pulling a clear thread for maneuvering solid-acid catalysts using carbons,which holds a novel promise for rationally functionalizing biochar-based catalysts for the remediation of macrolide antibiotics in polluted water.

关 键 词：Biochar engineering SULFONATION Heterogeneous catalysis Tylosin hydrolysis Antibiotic remediation 

分 类 号：O62[理学—有机化学] X703[理学—化学]