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In Situ Intermediates Determination and Cytotoxicological Assessment in Catalytic Oxidation of Formaldehyde: Implications for Catalyst Design and Selectivity Enhancement under Ambient Conditions

文献类型：期刊论文

作者Li, Haiwei2; Cui, Long2,3,4; Lu, Yanfeng3,4; Huang, Yu3,4; Cao, Junji3,4; Park, Duckshin1; Lee, Shun-cheng2; Ho, Wingkei5,6
刊名ENVIRONMENTAL SCIENCE & TECHNOLOGY
出版日期2019-05-07
卷号53期号:9页码:5230-5240
ISSN号0013-936X
DOI10.1021/acs.est.8b06234
通讯作者Lee, Shun-cheng(ceslee@polyu.edu.hk) ; Ho, Wingkei(keithho@eduhk.hk)
英文摘要Formation and decay of formaldehyde oxides (CH2OO) affect the complete oxidation of formaldehyde. However, the speciation and reactivity of CH2OO are poorly understood because of its extremely fast kinetics and indirect measurements. Herein, three isomers of CH2OO (i.e., main formic acid, small dioxirane, and minor CH2OO Criegee) were in situ determined and confirmed as primary intermediates of the room-temperature catalytic oxidation of formaldehyde with two reference catalysts, that is, TiO2/MnOx-CeO2 and Pt/MnOx-CeO2. CH2OO Criegee is quite reactive, whereas formic acid and dioxirane have longer lifetimes. The production, stabilization, and removal of the three intermediates are preferentially performed at high humidity, matching well with the decay rate of CH2OO at approximately 6.6 x 10(3) s(-1) in humid feed gas faster than 4.0 x 103 s(-1) in dry feed. By contrast, given that a thinner water/TiO2 interface was well-defined in TiO2/MnOx-CeO2, fewer reductions in the active sites and catalytic activity were found when humidity was decreased. Furthermore, lethal intermediates mostly captured at the TiO2/MnOx-CeO2 surface suppressed the toxic off-gas emissions. This study provides practical insights into the rational design and selectivity enhancement of a reliable catalytic process for indoor air purification under unfavorable ambient conditions.
WOS关键词SIMPLEST CRIEGEE INTERMEDIATE ; ROOM-TEMPERATURE ; WATER ; TIO2 ; HYDROPHILICITY ; NANOPARTICLES ; REACTIVITY ; REMOVAL ; VACANCY ; CHARGE
资助项目National Key Research and Development Program of China[2016YFA0203000] ; Research Grants Council of Hong Kong Government[T24/504/17] ; Research Grants Council of Hong Kong Government[PolyU152083/14E] ; Research Grants Council of Hong Kong Government[PolyU152090/15E] ; Research Grants Council of Hong Kong Government[GRF 18301117] ; Hong Kong RGC Collaborative Research Fund[C5022 -14G] ; Dean's Reserved Fund, FLASS from EdUHK[04360] ; IRG from EdUHK[R4016]
WOS研究方向Engineering ; Environmental Sciences & Ecology
语种英语
WOS记录号WOS:000467641800061
出版者AMER CHEMICAL SOC
资助机构National Key Research and Development Program of China ; Research Grants Council of Hong Kong Government ; Hong Kong RGC Collaborative Research Fund ; Dean's Reserved Fund, FLASS from EdUHK ; IRG from EdUHK
源URL[http://ir.ieecas.cn/handle/361006/14085]  
专题地球环境研究所_粉尘与环境研究室
通讯作者Lee, Shun-cheng; Ho, Wingkei
作者单位1.Korea Railrd Res Inst, Transportat Environm Res Team, Uiwan Si, Gyeonggi Do, South Korea
2.Hong Kong Polytech Univ, Dept Civil & Environm Engn, Hong Kong, Peoples R China
3.Chinese Acad Sci, Inst Earth Environm, SKLLQG, Xian 710061, Shaanxi, Peoples R China
4.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, Xian 710061, Shaanxi, Peoples R China
5.Educ Univ Hong Kong, Dept Sci & Environm Studies, Hong Kong, Peoples R China
6.City Univ Hong Kong, State Key Lab Marine Pollut, Hong Kong, Peoples R China
推荐引用方式
GB/T 7714		 Li, Haiwei,Cui, Long,Lu, Yanfeng,et al. In Situ Intermediates Determination and Cytotoxicological Assessment in Catalytic Oxidation of Formaldehyde: Implications for Catalyst Design and Selectivity Enhancement under Ambient Conditions[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2019,53(9):5230-5240.
APA Li, Haiwei.,Cui, Long.,Lu, Yanfeng.,Huang, Yu.,Cao, Junji.,...&Ho, Wingkei.(2019).In Situ Intermediates Determination and Cytotoxicological Assessment in Catalytic Oxidation of Formaldehyde: Implications for Catalyst Design and Selectivity Enhancement under Ambient Conditions.ENVIRONMENTAL SCIENCE & TECHNOLOGY,53(9),5230-5240.
MLA Li, Haiwei,et al."In Situ Intermediates Determination and Cytotoxicological Assessment in Catalytic Oxidation of Formaldehyde: Implications for Catalyst Design and Selectivity Enhancement under Ambient Conditions".ENVIRONMENTAL SCIENCE & TECHNOLOGY 53.9(2019):5230-5240.

入库方式： OAI收割

来源：地球环境研究所

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