机构:
Jozef Stefan Inst, Gaseous Elect, Jamova cesta 39, SI-1000 Ljubljana, SloveniaNatl Inst Chem, Dept Inorgan Chem & Technol, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
Zavasnik, Janez
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Tusar, Natasa Novak
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Natl Inst Chem, Dept Inorgan Chem & Technol, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
Univ Nova Gor, Vipavska ul 13, SI-5000 Nova Gorica, SloveniaNatl Inst Chem, Dept Inorgan Chem & Technol, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
To exploit the potential of both ZrO2 and CeO2, the mixed oxides with Ce content up to 5 wt.% were prepared via the simple coprecipitation method, subsequently loaded with Au catalysts, and investigated in the hydrogenation of CO2. The obtained catalysts, namely Au/ZrCex (x = nCe/nZr = 0.0-0.1), exhibit similar Au content (0.7 wt.%), structural and textural properties, however, considerably different acidic/basic properties and great surface oxygen vacancy. The introduction of Ce leads to slightly decreased CO2 conversion, which was found propor-tional to the Ce content. Interestingly, it is evidenced that the methanol selectivity is closely related to the acidic/ basic properties of the catalysts employed. Over the broad range of acid site density (ASD) ranging from 400 to 700 mu mol g-1, the highest methanol selectivity of 27 % was recorded at 250 degrees C and 40 bar over the catalyst exhibiting an ASD of 600 mu mol g-1, which decreased with further increasing ASD. The volcano-shape trend was also discovered for the base site density showing the critical point at 120 mu mol g-1 over the range from 90 to 210 mu mol g-1. These findings suggest that the acidic/basic properties can be tuned, e.g., via thermal treatment, to tailor the product distribution of the CO2 hydrogenation. Above all, the Au catalysts supported on ZrO2-CeO2 mixed oxides exhibit excellent catalytic stability, e.g., a methanol formation rate of 3.32 gCH3OH center dot (gAu center dot h)- 1 is remained over the reaction course of 93 h at 250 degrees C and 40 bar for Au/ZrCe0.025 sample.
机构:
Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and TechnologyKey Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology
沈茂
张昭
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Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and TechnologyKey Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology
张昭
贾发瑞
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Shanxi Irico Photo Electronic Material Corporation Research and Development DepartmentKey Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology
机构:
China Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Wang, Jianbing
Wang, Guoqing
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China Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Wang, Guoqing
Yang, Chunli
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China Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Yang, Chunli
Yang, Shaoxia
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North China Elect Power Univ, Sch Energy & Power Engn, Beijing 102206, Peoples R ChinaChina Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Yang, Shaoxia
Huang, Qing
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机构:
China Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China