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Correlations between the catalyst properties and catalytic activity of Au on ZrO2-CeO2 in the hydrogenation of CO2
被引:2
|作者:
Vu, Hue-Tong
[1
]
Finsgar, Matjaz
[2
]
Zavasnik, Janez
[3
]
Tusar, Natasa Novak
[1
,4
]
Pintar, Albin
[1
]
机构:
[1] Natl Inst Chem, Dept Inorgan Chem & Technol, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
[2] Univ Maribor, Fac Chem & Chem Engn, Smetanova 17, SI-2000 Maribor, Slovenia
[3] Jozef Stefan Inst, Gaseous Elect, Jamova cesta 39, SI-1000 Ljubljana, Slovenia
[4] Univ Nova Gor, Vipavska ul 13, SI-5000 Nova Gorica, Slovenia
关键词:
CO2;
utilization;
Au;
CeO2-ZrO2 mixed oxides;
AmorphousZrO2;
Methanol synthesis;
CARBON-DIOXIDE;
METHANOL SYNTHESIS;
HETEROGENEOUS CATALYSTS;
OXIDATION-STATE;
GOLD;
NANOPARTICLES;
SURFACE;
CERIA;
SELECTIVITY;
SUPPORT;
D O I:
10.1016/j.apsusc.2023.156737
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
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.
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页数:12
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