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
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.
