Preparation and Characterization of Modified-ZrO2 Catalysts for the Reaction of CO Hydrogenation

摘要/Abstract

摘要： ZrO2 in different structures and CexZr4-xO8 solid solutions have been prepared by a sol-gel related method with propionic acid as the solvent. The results of their characterization and CO hydro- genation performance evaluation show that t-ZrO2 has better catalytic performance for CO hydrogenation to hydrocarbon than m-ZrO2. Cerium (III) acetate and zirconium (IV) acetylacetonate have been chosen as the most suitable starting materials for CexZr4-xO8 solid solution preparation. Ce-Zr reducibility prop- erties are increased by the incorporation of zirconium oxide in the ceria structure. Ce2Zr2O8 exhibits a higher activity, lower methane selectivity and higher iso-C4 selectivity than tetragonal ZrO2. This implies that the formation mechanism of C4 hydrocarbons, especially that for the iso-C4 fraction is different over Ce2Zr2O8 and t-ZrO2.

关键词: CexZr4-xO8, solid solution, sol-gel related method, carbon monoxide, hydrogenation, hydrocarbons

Abstract: ZrO2 in different structures and CexZr4-xO8 solid solutions have been prepared by a sol-gel related method with propionic acid as the solvent. The results of their characterization and CO hydro- genation performance evaluation show that t-ZrO2 has better catalytic performance for CO hydrogenation to hydrocarbon than m-ZrO2. Cerium (III) acetate and zirconium (IV) acetylacetonate have been chosen as the most suitable starting materials for CexZr4-xO8 solid solution preparation. Ce-Zr reducibility prop- erties are increased by the incorporation of zirconium oxide in the ceria structure. Ce2Zr2O8 exhibits a higher activity, lower methane selectivity and higher iso-C4 selectivity than tetragonal ZrO2. This implies that the formation mechanism of C4 hydrocarbons, especially that for the iso-C4 fraction is different over Ce2Zr2O8 and t-ZrO2.

Key words: CexZr4-xO8, solid solution, sol-gel related method, carbon monoxide, hydrogenation, hydrocarbons

Qingjie Ge;A. Kiennemann;A. C. Roger;Wenzhao Li;Hengyong Xu. Preparation and Characterization of Modified-ZrO2 Catalysts for the Reaction of CO Hydrogenation[J]. 能源化学(英文), 2004, 13 (1): 41-44.

Qingjie Ge;A. Kiennemann;A. C. Roger;Wenzhao Li;Hengyong Xu. Preparation and Characterization of Modified-ZrO2 Catalysts for the Reaction of CO Hydrogenation[J]. Journal of Energy Chemistry, 2004, 13 (1): 41-44.

[1]	Weiwei Wang, Zhenping Qu, Lixin Song, Qiang Fu. An investigation of Zr/Ce ratio influencing the catalytic performance of CuO/Ce_1-xZr_xO₂ catalyst for CO₂ hydrogenation to CH₃OH[J]. 能源化学(英文版), 2020, 47(8): 18-28.
[2]	Zhong-Pan Hu, Yansu Wang,dandan Yang, Zhong-Yong Yuan. CrO_x supported on high-silica HZSM-5 for propane dehydrogenation[J]. 能源化学(英文版), 2020, 47(8): 225-233.
[3]	Munjeong Jang, Byeong Soo Shin, Young Suk Jo, Jeong Won Kang, Sang Kyu Kwak, Chang Won Yoon, Hyangsoo Jeong. A study on hydrogen uptake and release of a eutectic mixture of biphenyl and diphenyl ether[J]. 能源化学(英文版), 2020, 42(3): 11-16.
[4]	Qinqin Yu, Tie Yu, Hongyu Chen, Guangzong Fang, Xiulian Pan, Xinhe Bao. The effect of Al³⁺ coordination structure on the propane dehydrogenation activity of Pt/Ga/Al₂O₃ catalysts[J]. 能源化学(英文版), 2020, 41(2): 93-99.
[5]	Ming Yang, Xile Xing, Ting Zhu, Xuedi Chen, Yuan Dong, Hansong Cheng. Fast hydrogenation kinetics of acridine as a candidate of liquid organic hydrogen carrier family with high capacity[J]. 能源化学(英文版), 2020, 41(2): 115-119.
[6]	Yujun Zhao, Huanhuan Zhang, Yuxi Xu, Shengnian Wang, Yan Xu, Shengping Wang, Xinbin Ma. Interface tuning of Cu⁺/Cu⁰ by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO₂ catalyst[J]. 能源化学(英文版), 2020, 49(10): 248-256.
[7]	Weiwei Wang, Zhenping Qu, Lixin Song, Qiang Fu. CO₂ hydrogenation to methanol over Cu/CeO₂ and Cu/ZrO₂ catalysts: Tuning methanol selectivity via metal-support interaction[J]. 能源化学(英文版), 2020, 40(1): 22-30.
[8]	Hongen Yu, Xue Yang, Yong Wu, Yanru Guo, Shuan Li, Wei Lin, Xingguo Li, Jie Zheng. Bimetallic Ru-Ni/TiO₂ catalysts for hydrogenation of N-ethylcarbazole: Role of TiO₂ crystal structure[J]. 能源化学(英文版), 2020, 40(1): 188-195.
[9]	Igor Orlowski, Mark Douthwaite, Sarwat Iqbal, James S. Hayward, Thomas E. Davies, Jonathan K. Bartley, Peter J. Miedziak, Jun Hirayama, David J. Morgan, David J. Willock, Graham J. Hutchings. The hydrogenation of levulinic acid to γ-valerolactone over Cu-ZrO₂ catalysts prepared by a pH-gradient methodology[J]. 能源化学(英文版), 2019, 36(9): 15-24.
[10]	Lingling Shui, Guoxiu Zhang, Bin Hu, Xingxing Chen, Mingliang Jin, Guofu Zhou, Nan Li, Martin Muhler, Baoxiang Peng. Photocatalytic one-step synthesis of Ag nanoparticles without reducing agent and their catalytic redox performance supported on carbon[J]. 能源化学(英文版), 2019, 36(9): 37-46.
[11]	Maryam Kiani, Jie Zhang, Yan Luo, Yihan Chen, Jinwei Chen, Jinlong Fan, Gang Wang, Ruilin Wang. Facile synthesis and enhanced catalytic activity of electrochemically dealloyed platinum-nickel nanoparticles towards formic acid electro-oxidation[J]. 能源化学(英文), 2019, 28(8): 9-16.
[12]	Adhitya G. Saputro, Refaldi I. D. Putra, Arifin L. Maulana, Muhammad U. Karami, Mochamad R. Pradana, Mohammad K. Agusta, Hermawan K. Dipojono, Hideaki Kasai. Theoretical study of CO₂ hydrogenation to methanol on isolated small Pd_x clusters[J]. 能源化学(英文), 2019, 28(8): 79-87.
[13]	Fei Huang, Zhimin Jia, Jiangyong Diao, Hua Yuan, Dangsheng Su, Hongyang Liu. Palladium nanoclusters immobilized on defective nanodiamondgraphene core-shell supports for semihydrogenation of phenylacetylene[J]. 能源化学(英文), 2019, 28(6): 31-36.
[14]	Chuntao Zhang, Zhibao Huo, Dezhang Ren, Zhiyuan Song, Yunjie Liu, Fangming Jin, Wanning Zhou. Catalytic transfer hydrogenation of levulinate ester into γ -valerolactone over ternary Cu/ZnO/Al₂O₃ catalyst[J]. 能源化学(英文), 2019, 28(5): 189-197.
[15]	Kai Tie, Xiulian Pan, Tie Yu, Pan Li, Limin He, Xinhe Bao. A highly active and stable Pd/B-doped carbon catalyst for the hydrogenation of 4-carboxybenzaldehyde[J]. 能源化学(英文), 2019, 28(4): 154-158.