Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare ...Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.展开更多
Three reactions involved in dimethyl ether (DME) synthesis from COhydrogenation: methanol synthesis reaction (MSR), methanol dehydration reaction (MDR) and water gasshift reaction (WGSR) are studied by thermodynamic c...Three reactions involved in dimethyl ether (DME) synthesis from COhydrogenation: methanol synthesis reaction (MSR), methanol dehydration reaction (MDR) and water gasshift reaction (WGSR) are studied by thermodynamic calculation. For demonstrating this process indetail, three models, MSR, MSR+MDR, MSR+MDR+WGSR, are used. Their basic characteristics can beobtained by varying widely the ratios of H_2 to CO in the feed (no CO_2). Through thermodynamicanalysis a chemical synergic effect obviously exists in the second and third models. By comparisonbetween two models it is found that WGSR plays a special role in dimethyl ether synthesis. It ispossible for the two models to shift one to the other by regulating CO_2 concentration in feed. ForModel 2, the selectivity for DME in oxygenates (DME+methanol) does not change with the ratio of H_2to CO.展开更多
文摘Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.
基金This work is supported by the National High Technology Research and Development Program of China (Grant: 2002AA529070).
文摘Three reactions involved in dimethyl ether (DME) synthesis from COhydrogenation: methanol synthesis reaction (MSR), methanol dehydration reaction (MDR) and water gasshift reaction (WGSR) are studied by thermodynamic calculation. For demonstrating this process indetail, three models, MSR, MSR+MDR, MSR+MDR+WGSR, are used. Their basic characteristics can beobtained by varying widely the ratios of H_2 to CO in the feed (no CO_2). Through thermodynamicanalysis a chemical synergic effect obviously exists in the second and third models. By comparisonbetween two models it is found that WGSR plays a special role in dimethyl ether synthesis. It ispossible for the two models to shift one to the other by regulating CO_2 concentration in feed. ForModel 2, the selectivity for DME in oxygenates (DME+methanol) does not change with the ratio of H_2to CO.
