CAS OpenIR
Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways
Zhong, Chen1,2; Zhao, He2; Cao, Hongbin1,2; Fu, Jun3; Xie, Yongbing2; Sun, Zhi2
2019-03-01
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume359Pages:518-529
Abstract

Manganese dioxides (MnO2) govern the polymerization of phenolic and anilinic pollutants in nature water body. The studies on the chemistry of different phases of MnO2 was relatively limited. Here we compared two MnO2, layer delta-MnO2 and tunnel gamma-MnO2, on their reaction kinetics and removal pathways with acetaminophen (APAP) as model compound. We found the kinetics of acetaminophen transformation by MnO2 were largely influenced by pH values and MnO2 structures. In neutral systems, APAP removal by delta-MnO2 was faster than by gamma-MnO2. This was attributed to the higher catalytic potential of delta-MnO2. In acidic systems, APAP removal by gamma-MnO2 was faster than by delta-MnO2. This was attributed to the larger surface area and weaker electrostatic repulsion of gamma-MnO2 to APAP in acidic conditions. Furthermore, the pathways of acetaminophen transformation were influenced by pH values. Dimerization and hydrolysis-oxidation were the two major APAP transformation pathways by both MnO2 in neutral and acidic systems. Low pH values induced the nucleophilic addition between quinoneimine (the product of hydrolysis-oxidation) and anilines (e.g., APAP and its dimers). Low pH values also promoted the dimerization degrees of APAP. The hydrophilicity of APAP transformation products by MnO2 were significantly reduced by low pH values. This work reconsidered the significances of acidity in the pollutants transformation by MnO2, and provided new perspectives to study the pollutants transformation by different phases of MnO2.

KeywordBirnessite (Delta-mno2) Gamma-mno2 Kinetics Dimerization Nucleophilic Addition
DOI10.1016/j.cej.2018.11.172
Language英语
WOS KeywordManganese Oxide ; Humic-acid ; Oxidation ; Water ; Degradation ; Dioxide ; Products ; Ion ; Tetrabromobisphenol ; Reactivity
Funding ProjectNational Key Research and Development Program of China[2017YFB0403305] ; National Natural Science Foundation of China[51425405] ; National Natural Science Foundation of China[51378487] ; Youth Innovation Promotion Association, CAS[2014037]
WOS Research AreaEngineering
WOS SubjectEngineering, Environmental ; Engineering, Chemical
Funding OrganizationNational Key Research and Development Program of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association, CAS
WOS IDWOS:000454137400051
PublisherELSEVIER SCIENCE SA
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/27678
Collection中国科学院过程工程研究所
Corresponding AuthorZhao, He
Affiliation1.Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing Engn Res Ctr Proc Pollut Control, Beijing 100190, Peoples R China
3.Sino Japan Friendship Ctr Environm Protect, Beijing 100029, Peoples R China
Recommended Citation
GB/T 7714
Zhong, Chen,Zhao, He,Cao, Hongbin,et al. Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways[J]. CHEMICAL ENGINEERING JOURNAL,2019,359:518-529.
APA Zhong, Chen,Zhao, He,Cao, Hongbin,Fu, Jun,Xie, Yongbing,&Sun, Zhi.(2019).Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways.CHEMICAL ENGINEERING JOURNAL,359,518-529.
MLA Zhong, Chen,et al."Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways".CHEMICAL ENGINEERING JOURNAL 359(2019):518-529.
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