Organic acid-assisted preparation of highly dispersed Co/ZrO2 catalysts with superior activity for CO2 methanation | |
Li, Wenhui2; Liu, Yi2; Mu, Minchen2; Ding, Fanshu2; Liu, Zhongmin3; Guo, Xinwen2; Song, Chunshan1,2,4 | |
刊名 | APPLIED CATALYSIS B-ENVIRONMENTAL |
2019-10-05 | |
卷号 | 254页码:531-540 |
关键词 | CO2 methanation Cobalt catalyst ZrO2 Organic acid High dispersion |
ISSN号 | 0926-3373 |
DOI | 10.1016/j.apcatb.2019.05.028 |
通讯作者 | Guo, Xinwen(guoxw@dlut.edu.cn) ; Song, Chunshan(csong@psu.edu) |
英文摘要 | Various organic acids were investigated for preparing the highly dispersed cobalt catalysts on zirconia support, Co/ZrO2, by an acid-assisted incipient wetness impregnation. The organic acid-assisted preparation results in highly dispersed Co/ZrO2 catalysts which demonstrate superior catalytic activity with only 2 wt.% Co loading for CO2 methanation. Among the acids, the carboxylic acids with bigger molecular weight, more carboxyl groups and hydroxyl groups are more effective. Furthermore, the amino acids can also change the charge property of ZrO2 surface through controlling the solution pH and increase the metal dispersion through strong electrostatic adsorption. It is worth mentioning that, among the numerous organic acids, citric acid-assisted preparation gives Co/ZrO2 catalyst with superior catalytic activity and increased the CO2 conversion from 38% to 85% with highest turnover frequency. The linear relationship between metal dispersion and TOF with the molar ratio of acid to cobalt n(CA/Co) ranging from 0 to 2 demonstrates the importance of well dispersed metal particles in the enhanced activity. However, when the n(CA/Co) value exceeds 2 and the metal particle size further decreases, but no further enhancement is observed and the CO2 conversion even slightly decreased at the n(CA/Co) value of 5. The organic acids-assisted strategy can lead to increased metal dispersion and higher TOF for Co/ZrO(2 )catalysts; the appropriate metal dispersion corresponds to the suitable Co/ZrO2 interaction with oxygen vacancy which leads to more catalytically active sites for CO2 adsorption and catalytic hydrogenation. The organic acid-assisted strategy provides a new design approach for highly dispersed and active catalysts. |
资助项目 | National Key Research and Development Program of China[2016YFB0600902-5] ; National Natural Science Foundation of China[21503029] |
WOS关键词 | SUPPORTED COBALT CATALYSTS ; FISCHER-TROPSCH SYNTHESIS ; LOW-TEMPERATURE ; CARBON-DIOXIDE ; CITRIC-ACID ; MICROSCOPIC OBSERVATIONS ; SELECTIVE METHANATION ; TIO2 PHOTOCATALYSTS ; CO/AL2O3 CATALYSTS ; OXIDATION-STATE |
WOS研究方向 | Chemistry ; Engineering |
语种 | 英语 |
出版者 | ELSEVIER SCIENCE BV |
WOS记录号 | WOS:000472697500053 |
资助机构 | National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China |
内容类型 | 期刊论文 |
源URL | [http://cas-ir.dicp.ac.cn/handle/321008/175721] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
通讯作者 | Guo, Xinwen; Song, Chunshan |
作者单位 | 1.Penn State Univ, Clean Fuels & Catalysis Program, PSU DUT Joint Ctr Energy Res, EMS Energy Inst,Dept Energy & Mineral Engn, University Pk, PA 16802 USA 2.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 4.Penn State Univ, Clean Fuels & Catalysis Program, PSU DUT Joint Ctr Energy Res, EMS Energy Inst,Dept Chem Engn, University Pk, PA 16802 USA |
推荐引用方式 GB/T 7714 | Li, Wenhui,Liu, Yi,Mu, Minchen,et al. Organic acid-assisted preparation of highly dispersed Co/ZrO2 catalysts with superior activity for CO2 methanation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,254:531-540. |
APA | Li, Wenhui.,Liu, Yi.,Mu, Minchen.,Ding, Fanshu.,Liu, Zhongmin.,...&Song, Chunshan.(2019).Organic acid-assisted preparation of highly dispersed Co/ZrO2 catalysts with superior activity for CO2 methanation.APPLIED CATALYSIS B-ENVIRONMENTAL,254,531-540. |
MLA | Li, Wenhui,et al."Organic acid-assisted preparation of highly dispersed Co/ZrO2 catalysts with superior activity for CO2 methanation".APPLIED CATALYSIS B-ENVIRONMENTAL 254(2019):531-540. |
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