d Lewis acid transformation;
Hydrogen spillover;
Non-reducible oxides;
Reducible oxides;
Ammonia migration;
SPILLOVER;
PLATINUM;
CATALYST;
MIGRATION;
ZEOLITES;
PYRIDINE;
AMMONIA;
GAS;
D O I:
10.1007/s11244-018-0995-1
中图分类号:
O69 [应用化学];
学科分类号:
081704 ;
摘要:
The Lewis acid transformation to Bronsted acid was investigated over the Pt/gamma-Al2O3 hybrid catalysts in the presence of hydrogen atmosphere by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of adsorbed NH3. The changes of FTIR spectra were monitored during the introduction of hydrogen at 40 degrees C and atmospheric pressure for 130 min. The degrees of Lewis acid transformation were varied by addition of non-reducible (SiO2 and Al2O3) and reducible (ZrO2, TiO2 and CeO2) oxides to the Pt/gamma-Al2O3 catalysts as the hybrid catalysts. According to the in situ DRIFTS, the hydrogen temperature programmed reduction (H-2-TPR), and the hydrogen temperature programmed desorption (H-2-TPD) results, the introduction of hydrogen resulted in a decrease in the amount of ammonia adsorbed on Lewis acid sites, and an increase in the amount of ammonium ions on Bronsted acid sites with time on stream. It is proposed that ammonia migration from Lewis acid sites to Bronsted acid sites occurred during the introduction of hydrogen in the presence of Pt particles when compared to the observation of only observed catalysts (without Pt particles). The addition of reducible oxides led to the high rate of Lewis acid transformation, which was higher than those of the non-reducible oxides. Weaker Lewis acid sites and higher amount of hydrogen spillover over the observed catalysts enhanced the rate of Lewis acid transformation in this study. However, the amount of Lewis acid sites at the initial stage did not play an important role in these transformations.
机构:Chulalongkorn University,Department of Chemical Engineering, Faculty of Engineering, Center of Excellence on Catalysis and Catalytic Reaction Engineering
Adisak Guntida
Kongkiat Suriye
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机构:Chulalongkorn University,Department of Chemical Engineering, Faculty of Engineering, Center of Excellence on Catalysis and Catalytic Reaction Engineering
Kongkiat Suriye
Joongjai Panpranot
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机构:Chulalongkorn University,Department of Chemical Engineering, Faculty of Engineering, Center of Excellence on Catalysis and Catalytic Reaction Engineering
Joongjai Panpranot
Piyasan Praserthdam
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机构:Chulalongkorn University,Department of Chemical Engineering, Faculty of Engineering, Center of Excellence on Catalysis and Catalytic Reaction Engineering
机构:
Qilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China
Han, Shiwang
Xuan, Chengbo
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Qilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China
Xuan, Chengbo
Wang, Luyuan
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Qilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China
Wang, Luyuan
Zhang, Xingyu
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机构:
Qilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China
Zhang, Xingyu
Shao, Ranlei
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机构:
Qilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China
Shao, Ranlei
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机构:
Cheng, Xingxing
Wang, Zhiqiang
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机构:
Shandong Univ, Natl Engn Lab Coal Fired Pollutants Emiss Reduct, Shandong Prov Key Lab Energy Carbon Reduct & Resou, Jinan 250061, Peoples R ChinaQilu Univ Technol, Shandong Acad Sci, Energy Res Inst, Jinan 250014, Peoples R China