The catalytic role of nascent Cu(OH)(2) particles in the sulfite-induced oxidation of organic contaminants

doi:10.1016/j.cej.2019.01.114

	The catalytic role of nascent Cu(OH)(2) particles in the sulfite-induced oxidation of organic contaminants
	Wu, Feng 4; Li, Jinjun 4; Luo, Liting 1; Zhou, Danna 2,3; Yuan, Yanan 4; Luo, Tao 4
刊名	CHEMICAL ENGINEERING JOURNAL
	2019-05-01
卷号	363 页码:329-336
关键词	Cupric hydroxide Sulfite autoxidation Oxysulfur radical Paracetamol Alkaline pH Surface complexation
ISSN号	1385-8947
DOI	10.1016/j.cej.2019.01.114
英文摘要	In the recent years, sulfite-induced oxidation of various contaminants using oxysulfur radicals (SO4 center dot-, SO5 center dot- and SO3 center dot-) has been explored to establish novel advanced oxidation processes (AOPs). Although transition metals, such as cupric ions (Cu(II)), have been demonstrated to be capable of activating sulfite (S(IV)), the catalytic mechanism of the specific Cu(II) species is still not very clear. In this work, N-acetyl-para-aminophenol (APAP) was used as a basic substrate to investigate the process, mechanism and stability of the Cu(II)-S(IV) system with low dosages of Cu(II) (0.010 mmol L-1) in an alkaline solution (pH 10). The results show that 0.010 mmol L-1 Cu(II) can efficiently activate S(IV) for the oxidation of APAP and other contaminants (e.g., metoprolol, sulfanilamide, aniline, 4-chloroaniline, N,N-dimethylaniline, p-nitrophenol and 3-nitrophenol). Simulation calculations for the distribution of the Cu(II) species and pH-dependence of APAP oxidation in the Cu(II)-S(IV) system showed that Cu(OH)(2) particles are the major active species in the catalysis of S(IV). The surface complexation of S(IV) with the Cu(OH)(2) particles prior to the production of oxysulfur radicals is the basic mechanism of the alkaline Cu(II)-S(IV) system. Radical inhibition with scavengers (ethanol, tert-butyl alcohol or aniline) demonstrates that SO5 center dot-, SO4 center dot- and hydroxyl radicals (HO center dot) are responsible for the contaminant oxidation. Moreover, SO5 center dot- is believed to be the main active species in the Cu(II)-S(IV) system, which has a second-order rate constant of 2.98 x 10(8)M(-1) s(-1) with APAP. This work renews our recognition of the Cu(II)-S(IV) system applications and further understanding of the catalytic role of the nascent Cu(OH)(2) particles in the activation of S(IV).
资助项目	Science and Technology Planning Project of Guangdong Province[2017B030314092] ; National Natural Science Foundation of China[21876160]
WOS关键词	DRIVEN PHOTOCATALYTIC DEGRADATION ; ACTIVATED PERSULFATE OXIDATION ; ION SULFUR(IV) CHEMISTRY ; ACID ORANGE 7 ; RADICAL GENERATION ; ELECTRON-TRANSFER ; AQUEOUS-SOLUTIONS ; RATE CONSTANTS ; SYSTEM ; KINETICS
WOS研究方向	Engineering
语种	英语
出版者	ELSEVIER SCIENCE SA
WOS记录号	WOS:000457866400033
资助机构	Science and Technology Planning Project of Guangdong Province ; Science and Technology Planning Project of Guangdong Province ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Planning Project of Guangdong Province ; Science and Technology Planning Project of Guangdong Province ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Planning Project of Guangdong Province ; Science and Technology Planning Project of Guangdong Province ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Planning Project of Guangdong Province ; Science and Technology Planning Project of Guangdong Province ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/14328]
专题	中国科学院武汉物理与数学研究所
通讯作者	Wu, Feng; Luo, Liting
作者单位	1.Chinese Acad Sci, Wuhan Inst Phys & Math, Natl Ctr Magnet Resonance Wuhan, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China 2.China Univ Geosci, Fac Mat Sci & Chem, Wuhan 430074, Hubei, Peoples R China 3.Guangdong Inst Ecoenvironm Sci Technol, Guangdong Key Lab Agro Environm Pollut Control &, Guangzhou 510650, Guangdong, Peoples R China 4.Wuhan Univ, Sch Resources & Environm Sci, Wuhan 430079, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Wu, Feng,Li, Jinjun,Luo, Liting,et al. The catalytic role of nascent Cu(OH)(2) particles in the sulfite-induced oxidation of organic contaminants[J]. CHEMICAL ENGINEERING JOURNAL,2019,363:329-336.
APA	Wu, Feng,Li, Jinjun,Luo, Liting,Zhou, Danna,Yuan, Yanan,&Luo, Tao.(2019).The catalytic role of nascent Cu(OH)(2) particles in the sulfite-induced oxidation of organic contaminants.CHEMICAL ENGINEERING JOURNAL,363,329-336.
MLA	Wu, Feng,et al."The catalytic role of nascent Cu(OH)(2) particles in the sulfite-induced oxidation of organic contaminants".CHEMICAL ENGINEERING JOURNAL 363(2019):329-336.