Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways

doi:10.1016/j.cej.2018.11.172

	Acidity induced fast transformation of acetaminophen by different MnO2: Kinetics and pathways
	Zhong, Chen 1,2; Zhao, He 2; Cao, Hongbin 1,2; Fu, Jun 3; Xie, Yongbing 2; Sun, Zhi 2
刊名	CHEMICAL ENGINEERING JOURNAL
	2019-03-01
卷号	359 页码:518-529
关键词	Birnessite (delta-MnO2) gamma-MnO2 Kinetics Dimerization Nucleophilic addition
ISSN号	1385-8947
DOI	10.1016/j.cej.2018.11.172
英文摘要	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.
资助项目	National 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关键词	MANGANESE OXIDE ; HUMIC-ACID ; OXIDATION ; WATER ; DEGRADATION ; DIOXIDE ; PRODUCTS ; ION ; TETRABROMOBISPHENOL ; REACTIVITY
WOS研究方向	Engineering
语种	英语
出版者	ELSEVIER SCIENCE SA
WOS记录号	WOS:000454137400051
资助机构	National Key Research and Development Program of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association, CAS
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/27677]
专题	中国科学院过程工程研究所
通讯作者	Zhao, He
作者单位	1.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
推荐引用方式 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.