Heterogeneous catalytic reaction of SO2 on the surface of ultrafine Fe3O4 particle by XANES

Dan ZHANG; Bing WANG; Shanshan LIANG; Lei ZHENG; Weiyue FENG

doi:10.11889/j.0253-3219.2018.hjs.41.050101

您当前的位置：

首页 >

文章列表页 >

Heterogeneous catalytic reaction of SO₂ on the surface of ultrafine Fe₃O₄ particle by XANES

SYNCHROTRON RADIATION TECHNOLOGY AND APPLICATIONS | 更新时间：2021-05-19

- Heterogeneous catalytic reaction of SO₂ on the surface of ultrafine Fe₃O₄ particle by XANES
- NUCLEAR TECHNIQUES Vol. 41, Issue 5, Article number: 050101(2018)
- 作者机构：
  
  1.中国科学院高能物理研究所纳米生物效应与安全性院重点实验室北京 100049
  2.中国科学院大学北京 100049
  3.安徽大学健康科学研究院合肥 230601
  4.中国科学院高能物理研究所北京同步辐射装置北京 100049
- 作者简介：
- 基金信息：
  
  Key Program of Joint Funds of National Natural Science Foundation of China;National Natural Science Foundation of China;National Natural Science Foundation of China
- DOI：10.11889/j.0253-3219.2018.hjs.41.050101
  CLC： TL99;O434.1;O433.51;X513
- Received：01 December 2017，
  
  Revised：30 January 2018，
  
  Published：10 May 2018
- 稿件说明：
移动端阅览
Dan ZHANG, Bing WANG, Shanshan LIANG, et al. Heterogeneous catalytic reaction of SO₂ on the surface of ultrafine Fe₃O₄ particle by XANES[J]. Nuclear techniques, 2018, 41(5): 050101
DOI：

Dan ZHANG, Bing WANG, Shanshan LIANG, et al. Heterogeneous catalytic reaction of SO₂ on the surface of ultrafine Fe₃O₄ particle by XANES[J]. Nuclear techniques, 2018, 41(5): 050101 DOI： 10.11889/j.0253-3219.2018.hjs.41.050101.

摘要

超细颗粒物为大气中痕量气态污染物转化提供了广泛的反应界面，在其表面发生多相界面反应是大气二次颗粒物形成的主要途径。含铁超细颗粒是大气气溶胶的主要成分之一。本研究采用同步辐射X射线近边吸收谱（X-ray Absorption Near Edge Structure，XANES）技术开展了Fe

超细颗粒表面的多相反应研究，分析了反应时间、紫外照射及臭氧存在条件对二次颗粒物形成的影响。研究发现：SO

在Fe

超细颗粒表面能被快速氧化形成硫酸根（SO

），其中紫外光照（Ultra-Violet，UV）和O

可以促进硫酸根的生成。从反应时间上看，SO

在Fe

超细颗粒表面可快速反应生成高价态硫酸根，30 min时，约99%的硫化物转化成硫酸根。通过对S的XANES谱进行一阶导数处理，发现产物中还存在亚硫酸根（SO

）的峰，提示SO

在Fe

颗粒物表面可先生成亚硫酸根，进而被快速氧化成硫酸根。

Abstract

Background

Ultrafine particles (UFPs) may provide various micro-locations of heterogeneous chemical reactions of trace of gaseous substances in atmospheric environment. Iron-containing UFPs are the main components of atmospheric aerosol.

Purpose

This study aims to investigate heterogeneous reactions of SO

on Fe

UFPs.

Methods

S K-edge of products was investigated by synchrotron radiation X-ray absorption near edge structure (XANES).

Results

The results indicated that SO

could be rapidly oxidized to form sulfate on the surface of Fe

. Formation of sulfate can be promoted under the UV and O

conditions.

Conclusion

The formation of adsorbed sulfate likely involves the formation of pre-absorbed sulfite (SO

) and subsequent oxidation.

关键词

Keywords

references

S Yang , Y L Ma , F K Duan , . Characteristics and formation of typical winter haze in Handan, one of the most polluted cities in China . Science of the Total Environment , 2018 . 613-614 1367 - 1375 . DOI: 10.1016/j.scitotenv.2017.08.033 http://doi.org/10.1016/j.scitotenv.2017.08.033 .

P K Ma , P Zhang , J N Shu , . Characterization of secondary organic aerosol from photo-oxidation of gasoline exhaust and specific sources of major components . Environmental Pollution , 2018 . 232 65 - 72 . DOI: 10.1016/j.envpol.2017.09.018 http://doi.org/10.1016/j.envpol.2017.09.018 .

X Qiao , Q Ying , X H Li , . Source apportionment of PM 2.5 for 25 Chinese provincial capitals and municipalities using a source-oriented community multiscale air quality model . Science of the Total Environment , 2018 . 612 462 - 471 . DOI: 10.1016/j.scitotenv.2017.08.272 http://doi.org/10.1016/j.scitotenv.2017.08.272 .

Y Z Tian , J Y Liu , S Q Han , . Spatial, seasonal and diurnal patterns in physicochemical characteristics and sources of PM 2.5 in both inland and coastal regions within a megacity in China . Journal of Hazardous Materials , 2018 . 342 139 - 149 . DOI: 10.1016/j.jhazmat.2017.08.015 http://doi.org/10.1016/j.jhazmat.2017.08.015 .

R J Huang , Y L Zhang , C Bozzetti , . High secondary aerosol contribution to particulate pollution during haze events in China . Nature , 2014 . 514 ( 7521 ): 218 - 222 . DOI: 10.1038/nature13774 http://doi.org/10.1038/nature13774 .

C R Usher , A E Michel , V H Grassian . Reactions on mineral dust . Chemical Reviews , 2003 . 103 ( 12 ): 4883 - 4939 . DOI: 10.1021/cr020657y http://doi.org/10.1021/cr020657y .

马庆鑫 , 马金珠 , 楚碧武 , . 矿质和黑碳颗粒物表面大气非均相反应研究进展 . 科学通报 , 2015 . 60 ( 2 ): 122 - 136 . DOI: 10.1360/N972014-01190 http://doi.org/10.1360/N972014-01190 .

Qingxin MA , Jinzhu MA , Biwu CHU , . Current progress towards the heterogeneous reactions on mineral dust and soot . Chinese Science Bulletin , 2015 . 60 ( 2 ): 122 - 136 . DOI: 10.1360/N972014-01190 http://doi.org/10.1360/N972014-01190 .

J Y Park , M Jang . Heterogeneous photooxidation of sulfur dioxide in the presence of airborne mineral dust particles . Royal Society of Chemistry Advances , 2016 . 6 ( 63 ): 58617 - 58627 . DOI: 10.1039/c6ra09601h http://doi.org/10.1039/c6ra09601h .

H He , Y S Wang , Q X Ma , . Mineral dust and NO x promote the conversion of SO 2 to sulfate in heavy pollution days . Scientific Reports , 2014 . 4 ( 1 ): 4172 DOI: 10.1038/srep04172 http://doi.org/10.1038/srep04172 .

Z C Yu , M Jang , J Park . Modeling atmospheric mineral aerosol chemistry to predict heterogeneous photooxidation of SO 2 . Atmospheric Chemistry and Physics , 2017 . 17 ( 16 ): 10001 - 10017 . DOI: 10.5194/acp-17-10001-2017 http://doi.org/10.5194/acp-17-10001-2017 .

M Ullerstam , R Vogt , S Langer , . The kinetics and mechanism of SO 2 oxidation by O 3 on mineral dust . Physical Chemistry Chemical Physics , 2002 . 4 ( 19 ): 4694 - 4699 . DOI: 10.1039/b203529b http://doi.org/10.1039/b203529b .

C E Zubieta , L F Fortunato , P G Belelli , . Theoretical study of SO 2 adsorption on goethite (110) surface . Applied Surface Science , 2014 . 314 ( 10 ): 558 - 563 . DOI: 10.1016/j.apsusc.2014.06.147 http://doi.org/10.1016/j.apsusc.2014.06.147 .

Y Long , C C Zhang , X X Wang , . Oxidation of SO 2 to SO 3 catalyzed by graphene oxide foams . Journal of Materials Chemistry , 2011 . 21 ( 36 ): 13934 - 13941 . DOI: 10.1039/c1jm12031j http://doi.org/10.1039/c1jm12031j .

A R Ravishankara . Heterogeneous and multiphase chemistry in the troposphere . Science , 1997 . 276 ( 5315 ): 1058 - 1065 . DOI: 10.1126/science.276.5315.1058 http://doi.org/10.1126/science.276.5315.1058 .

Y Dupart , S M King , B Nekat . Mineral dust photochemistry induces nucleation events in the presence of SO 2 . Proceedings of the National Academy of Sciences , 2012 . 109 ( 51 ): 20842 - 20847 . DOI: 10.1073/pnas.1212297109 http://doi.org/10.1073/pnas.1212297109 .

D S Toledano , V E Henrich . Kinetics of SO 2 adsorption on photoexcited α-Fe 2 O 3 . Journal of Physical Chemistry B , 2001 . 105 ( 18 ): 3872 - 3877 . DOI: 10.1021/jp003327v http://doi.org/10.1021/jp003327v .

H B Fu , X Wang , H B Wu , . Heterogeneous uptake and oxidation of SO 2 on iron oxides . Journal of Physical Chemistry C , 2007 . 111 ( 16 ): 6077 - 6085 . DOI: 10.1021/jp070087b http://doi.org/10.1021/jp070087b .

俞淼 , 汪冰 , 张丹 , . SO 2 与CeO 2 超细颗粒非均相反应产物的细胞毒性效应 . 生态毒理学报 , 2017 . 12 ( 2 ): 63 - 70 . DOI: 10.7524/AJE.1673-5897.20170103004 http://doi.org/10.7524/AJE.1673-5897.20170103004 .

Miao YU , Bing WANG , Dan ZHANG , . Cytotoxicity study of secondary ultrafine particles forming from SO 2 reactionon CeO 2 ultrafine particles . Asian Journal of Ecotoxicology , 2017 . 12 ( 2 ): 63 - 70 . DOI: 10.7524/AJE.1673-5897.20170103004 http://doi.org/10.7524/AJE.1673-5897.20170103004 .

陆尔东 , 张新夷 . 固体表面结构的同步辐射研究:X射线吸收近边结构(XANES) . 物理学进展 , 1998 . 18 ( 3 ): 261 - 282 . http://kns.cnki.net/KCMS/detail/detail.aspx?filename=wlxj199803001&dbname=CJFD&dbcode=CJFQ .

Erdong LU , Xinyi ZHANG . Synchrotron radiation studies on solid surface structures:introduction to X-ray absorption near edge structure . Progress in Physics , 1998 . 18 ( 3 ): 261 - 282 . http://kns.cnki.net/KCMS/detail/detail.aspx?filename=wlxj199803001&dbname=CJFD&dbcode=CJFQ .

王荫淞 , 李爱国 , 魏仑 , . 用X射线吸收近边结构谱研究大气颗粒物中元素的种态 . 核技术 , 2004 . 27 ( 11 ): 810 - 813 . DOI: 10.3321/j.issn:0253-3219.2004.11.003 http://doi.org/10.3321/j.issn:0253-3219.2004.11.003 .

Yinsong WANG , Aiguo LI , Lun WEI , . Study on elemental speciation in airborne particulate matter by XANES . Nuclear Techniques , 2004 . 27 ( 11 ): 810 - 813 . DOI: 10.3321/j.issn:0253-3219.2004.11.003 http://doi.org/10.3321/j.issn:0253-3219.2004.11.003 .

冼鼎昌 . 北京同步辐射装置及其应用 , : 广西广西科学技术出版社 , 2016 .

Dingchang XIAN . Being synchrotron radiation facility and application , : Guangxi Guangxi Science and Technology Press , 2016 .

张龙力 , 王春岚 , 赵元生 , . 石油沥青质含硫结构的XANES导数光谱研究 . 燃料化学学报 , 2013 . 41 ( 11 ): 1328 - 1335 . http://www.oalib.com/paper/4967618 .

Longli ZHANG , Chunlan WANG , Yuansheng ZHAO , . Speciation and quantification of sulfur compounds in petroleum asphaltenes by derivative XANES spectra . Journal of Fuel Chemistry and Technology , 2013 . 41 ( 11 ): 1328 - 1335 . http://www.oalib.com/paper/4967618 .

G N George , M L Gorbaty . Sulfur K-edge X-ray absorption spectroscopy of petroleum asphaltenes and model compounds . Journal of the American Chemical Society , 1989 . 111 ( 9 ): 3182 - 3186 . DOI: 10.1021/ja00191a012 http://doi.org/10.1021/ja00191a012 .

Y F Cheng , G J Zheng , C Wei , . Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China . Science Advances , 2016 . 12 1 - 11 . DOI: 10.1126/sciadv.1601530 http://doi.org/10.1126/sciadv.1601530 .

H B Fu , T G Xu , S G Yang , . Photo induced formation of Fe(Ⅲ)-sulfato complexes on the surface of α-Fe 2 O 3 and their photochemical performance . Journal of Physical Chemistry C , 2009 . 113 ( 26 ): 11316 - 11322 . DOI: 10.1021/jp8088275 http://doi.org/10.1021/jp8088275 .

张秋菊 , 王晓 , 陈建民 , . SO 2 与Fe 2 O 3 生成Fe(Ⅱ)(aq)和硫酸盐的复相反应机理 . 高等学校化学学报 , 2006 . 27 ( 7 ): 1347 - 1350 . http://www.doc88.com/p-0137151270914.html .

Qiuju ZHANG , Xiao WANG , Jianmin CHEN , . Formation of Fe(Ⅱ)(aq) and sulfate via heterogeneous reaction of SO 2 with Fe 2 O 3 . Chemical Journal of Chinese Universities , 2006 . 27 ( 7 ): 1347 - 1350 . http://www.doc88.com/p-0137151270914.html .

M Setvín , U Aschauer , P Scheiber , . Reaction of O 2 with subsurface oxygen vacancies on TiO 2 anatase (101) . Science , 2013 . 341 ( 12 ): 988 - 990 . DOI: 10.1126/science.1239879 http://doi.org/10.1126/science.1239879 .

Y F Li , U Aschauer , J Chen , . Adsorption and reactions of O 2 on anatase TiO 2 . Accounts of Chemical Research , 2014 . 47 ( 11 ): 3361 - 3368 . DOI: 10.1021/ar400312t http://doi.org/10.1021/ar400312t .

J Baltrusaitis , D M Cwiertny , V H Grassian . Adsorption of sulfur dioxide on hematite and goethite particle surfaces . Physical Chemistry Chemical Physics , 2007 . 9 ( 41 ): 5542 - 5554 . DOI: 10.1039/b709167b http://doi.org/10.1039/b709167b .

D N Zhou , L Chen , C B Zhang , . A novel photochemical system of ferrous sulfite complex:kinetics and mechanisms of rapid decolorization of acid orange 7 in aqueous solutions . Water Research , 2014 . 57 ( 5 ): 87 - 95 . DOI: 10.1016/j.watres.2014.03.016 http://doi.org/10.1016/j.watres.2014.03.016 .

Views

下载量

CSCD

Alert me when the article has been cited

提交

Tools

Publicity Resources

Sulfur speciation in soil under long-term fertilization by XANES

Related Author

LIU Lijuan1 CUI Mingqi1 ZHAO Jia2 MA Yibing3 MA Chenyan1 ZHENG Lei1 ZHAO Yidong1 1

崔明启

赵佳

马义兵

马陈燕

郑雷

赵屹东

Related Institution

Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China) 2

北京工商大学机械工程学院

中国农业科学院农业资源与农业区划研究所

AI问答

Address：2019 Jialuo Road, Jiading, Shanghai, China Postal code：201800
Tel：021-39194977 Email：LHB@sinap.ac.cn
Technical support is provided by Beijing Founder electronics co., LTD 沪ICP备05005479号-1 京公网安备11010802024621
It is recommended to read the content of this site in Chrome&IE9+. Please switch to extreme mode in browser 360.
Cookies We use cookies to help provide and enhance our service and tailor content. By continuing, you agree to the use of cookies.
Total Visits：880473

⁰