A Novel Redox Precipitation to Synthesize Au-Doped α-MnO2 with High Dispersion toward Low-Temperature Oxidation of Formaldehyde

被引:185
作者
Chen, Jin [1 ,2 ]
Yan, Dongxu [1 ,2 ,3 ]
Xu, Zhen [1 ,2 ]
Chen, Xi [1 ,2 ,3 ]
Xu, Wenjian [1 ,2 ]
Jia, Hongpeng [1 ,2 ,3 ]
Chen, Jing [4 ,5 ,6 ]
机构
[1] Chinese Acad Sci, Inst Urban Environm, CAS Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
[2] Chinese Acad Sci, Inst Urban Environm, Key Lab Urban Pollutant Convers, Xiamen 361021, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, CAS Key Lab Design & Assembly Funct Nanostruct, Fujian Inst Res Struct Matter, Fuzhou 350002, Fujian, Peoples R China
[5] Chinese Acad Sci, Fujian Prov Key Lab Nanomat, Fujian Inst Res Struct Matter, Fuzhou 350002, Fujian, Peoples R China
[6] Chinese Acad Sci, Xiamen Inst Rare Earth Mat, Haixi Inst, Xiamen 361021, Peoples R China
基金
中国国家自然科学基金;
关键词
VOLATILE ORGANIC-COMPOUNDS; CATALYTIC-OXIDATION; ROOM-TEMPERATURE; CO OXIDATION; HETEROGENEOUS CATALYSIS; GASEOUS FORMALDEHYDE; AU/CEO2; CATALYSTS; MOLECULAR-OXYGEN; ACTIVATED CARBON; OXIDE CATALYSTS;
D O I
10.1021/acs.est.7b06039
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A novel method of redox precipitation was applied for the first time to synthesize a Au-doped alpha-MnO2 catalyst with high dispersion of the Au species. Au nano particles (NPs) can be downsized into approximate single atoms by this method, thereby realizing highly efficient utilization of Au element as well as satisfying low-temperature oxidation of formaldehyde (HCHO). Under catalysis of the optimal 0.25% Au/alpha-MnO2 catalyst, a polluted stream containing 500 ppm HCHO can be completely cleaned at 75 degrees C with the condition of a weight hourly space velocity (WHSV) of 60000 mL/(g h). Meanwhile, the catalyst retains good activity for removal of low-concentration HCHO (about 1 ppm) at ambient temperature with a high WHSV, and exhibits a high tolerance to water and long-term stability. Our characterization of Au/alpha-MnO2 and catalytic performance tests clearly demonstrate that the proper amount of Au doping facilitates formation of surface vacancy oxygen, lattice oxygen, and charged Au species as an active site, which are all beneficial to catalytic oxidation of HCHO. The oxidation of HCHO over Au-doped alpha-MnO2 catalyst obeys the Mars-van Krevelen mechanism as evidenced by in situ diffuse reflectance infrared Fourier transform spectroscopy.
引用
收藏
页码:4728 / 4737
页数:10
相关论文
共 64 条
[41]   Decomposition of gaseous formaldehyde in a photocatalytic reactor with a parallel array of light sources - 1. Fundamental experiment for reactor design [J].
Shiraishi, F ;
Ohkubo, D ;
Toyoda, K ;
Yamaguchi, S .
CHEMICAL ENGINEERING JOURNAL, 2005, 114 (1-3) :153-159
[42]  
Sun S., 2013, Scientific Reports, P3, DOI DOI 10.1038/SREP01775
[43]   Removal of low-concentration formaldehyde in air by DC corona discharge plasma [J].
Wan, Yajuan ;
Fan, Xing ;
Zhu, Tianle .
CHEMICAL ENGINEERING JOURNAL, 2011, 171 (01) :314-319
[44]   Catalytic behavior of supported Ru nanoparticles on the {100}, {110}, and {111} facet of CeO2 [J].
Wang, Fei ;
Li, Changming ;
Zhang, Xiaoyu ;
Wei, Min ;
Evans, David G. ;
Duan, Xue .
JOURNAL OF CATALYSIS, 2015, 329 :177-186
[45]   The effect of manganese vacancy in birnessite-type MnO2 on room-temperature oxidation of formaldehyde in air [J].
Wang, Jinlong ;
Li, Jinge ;
Jiang, Chuanjia ;
Zhou, Peng ;
Zhang, Pengyi ;
Yu, Jiaguo .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 204 :147-155
[46]   Study of catalytic decomposition of formaldehyde on Pt/TiO2 alumite catalyst at ambient temperature [J].
Wang, Lifeng ;
Sakurai, Makoto ;
Kameyama, Hideo .
JOURNAL OF HAZARDOUS MATERIALS, 2009, 167 (1-3) :399-405
[47]   The catalytic oxidation removal of low-concentration HCHO at high space velocity by partially crystallized mesoporous MnOx [J].
Wang, Min ;
Zhang, Lingxia ;
Huang, Weimin ;
Xiu, Tongping ;
Zhuang, Chenggang ;
Shi, Jianlin .
CHEMICAL ENGINEERING JOURNAL, 2017, 320 :667-676
[48]   Rational synthesis of α-MnO2 single-crystal nanorods [J].
Wang, X ;
Li, YD .
CHEMICAL COMMUNICATIONS, 2002, (07) :764-765
[49]   FeOx-supported platinum single-atom and pseudo-single-atom catalysts for chemoselective hydrogenation of functionalized nitroarenes [J].
Wei, Haisheng ;
Liu, Xiaoyan ;
Wang, Aiqin ;
Zhang, Leilei ;
Qiao, Botao ;
Yang, Xiaofeng ;
Huang, Yanqiang ;
Miao, Shu ;
Liu, Jingyue ;
Zhang, Tao .
NATURE COMMUNICATIONS, 2014, 5
[50]   Dynamic surface composition in a Mars-van Krevelen type reaction: CO oxidation on Au/TiO2 [J].
Widmann, D. ;
Behm, R. J. .
JOURNAL OF CATALYSIS, 2018, 357 :263-273