Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of nob...Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of noble metals.This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles(NPs)with the supported TiO_(2),achieving the moderate suppression of SMSI effects.The introduction of silica inhibits this encapsulation,as reflected in the characterization results such as XPS and HRTEM,while the Ti^(4+) to Ti^(3+) conversion due to SMSI can still be found on the support surface.Furthermore,the hydrogenation of cinnamaldehyde(CAL)as a probe reaction revealed that once this encapsulation behavior was suppressed,the adsorption capacity of the catalyst for small molecules like H_(2) and CO was enhanced,which thereby improved the catalytic activity and facilitated the hydrogenation of CAL.Meanwhile,the introduction of SiO_(2) also changed the surface structure of the catalyst,which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation.Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed.展开更多
A new type of transparent scratch resistant coatings including in-situ modified SiO2 (g-SiO2) in flame spray pyrolysis (FSP) process was prepared. The maximum content of g-SiO2 in the coating was 15 wt%, which is ...A new type of transparent scratch resistant coatings including in-situ modified SiO2 (g-SiO2) in flame spray pyrolysis (FSP) process was prepared. The maximum content of g-SiO2 in the coating was 15 wt%, which is higher than that of SiO2 modified by traditional wet chemical route (I-SiO2, only 10 wt%). The results of transmission electron microscopy have demonstrated that in-situ surface modified g-SiO2 particles dispersed well with smaller agglomerates in the final coating, which was much better than the particles modified via wet chemical route. Visible light transmittance and haze tests were introduced to characterize the optical quality of the films. All coatings were highly transparent with the visible light transmittance of above 80%, especially for coatings containing g-SiO2, which exhibited slightly higher visible light transmittance than l-SiO2 embedded one. The haze value of coatings incorporated with 15 wt% g-SiO2 was 1.85%, even lower than the coating with 5 wt% I-SiO2 (haze value of 2.09%), indicating much better clarity of g-SiO2. The excellent optical property of g-SiO2 filled coatings was attributed to the good dispersion and distribution of particles. Nano-indention and nano-scratch tests were con- ducted to investigate the scratch resistance of coatings on nano-scale. The surface hardness of the coatings rose by 18% and 14%, and the average friction coefficient decreased by 15% and 11%, respectively, compared to the neat coat due to the addition of 10 wt% g-SiO2 and I-SiO2. The pencil hardness of the coating with 15 wt% g-SiO2 increased from 2B for the neat coating to 2H. However, the pencil hardness of coating with 10 wt% I-SiO2 was only H. The results showed that the g-SiO2 embedded coatings exhibited higher scratch resistance and better optical properties.展开更多
Pd-based egg-shell nano-catalysts were prepared using porous hollow silica nanoparticles (PHSNs) as support, and the as-prepared catalysts were modified with TiO2 to promote their selectivity for hydro-genation of a...Pd-based egg-shell nano-catalysts were prepared using porous hollow silica nanoparticles (PHSNs) as support, and the as-prepared catalysts were modified with TiO2 to promote their selectivity for hydro-genation of acetylene. Pd nanoparticles were loaded evenly on PHSNs and TiO2 was loaded on the active Pd particles. The effects of reduction time and temperature and the amount of TiO2 added on catalytic per-formances were investigated by using a fixed-bed micro-reactor. It was found that the catalysts showed better performance when reduced at 300 ℃ than at 500℃, and if reduced for 1 h than 3 h. When the amount of Ti added was 6 times that of Pd, the catalyst showed the highest ethylene selectivity.展开更多
基金the National Natural Science Foundation of China(21576291,22003076)National Natural Science Foundation of China-Outstanding Youth foundation(22322814)the Fundamental Research Funds for the Central Universities(23CX03007A,22CX06012A)are gratefully acknowledge。
文摘Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of noble metals.This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles(NPs)with the supported TiO_(2),achieving the moderate suppression of SMSI effects.The introduction of silica inhibits this encapsulation,as reflected in the characterization results such as XPS and HRTEM,while the Ti^(4+) to Ti^(3+) conversion due to SMSI can still be found on the support surface.Furthermore,the hydrogenation of cinnamaldehyde(CAL)as a probe reaction revealed that once this encapsulation behavior was suppressed,the adsorption capacity of the catalyst for small molecules like H_(2) and CO was enhanced,which thereby improved the catalytic activity and facilitated the hydrogenation of CAL.Meanwhile,the introduction of SiO_(2) also changed the surface structure of the catalyst,which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation.Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed.
基金supported by the National Natural Science Foundation of China (Nos. 51173043, 21236003, and 21322607)the Basic Research Program of Shanghai (Nos. 13JC1408100 and 15JC1401300)+1 种基金the Key Scientific and Technological Program of Shanghai (No. 14521100800)the Fundamental Research Funds for the Central Universities.
文摘A new type of transparent scratch resistant coatings including in-situ modified SiO2 (g-SiO2) in flame spray pyrolysis (FSP) process was prepared. The maximum content of g-SiO2 in the coating was 15 wt%, which is higher than that of SiO2 modified by traditional wet chemical route (I-SiO2, only 10 wt%). The results of transmission electron microscopy have demonstrated that in-situ surface modified g-SiO2 particles dispersed well with smaller agglomerates in the final coating, which was much better than the particles modified via wet chemical route. Visible light transmittance and haze tests were introduced to characterize the optical quality of the films. All coatings were highly transparent with the visible light transmittance of above 80%, especially for coatings containing g-SiO2, which exhibited slightly higher visible light transmittance than l-SiO2 embedded one. The haze value of coatings incorporated with 15 wt% g-SiO2 was 1.85%, even lower than the coating with 5 wt% I-SiO2 (haze value of 2.09%), indicating much better clarity of g-SiO2. The excellent optical property of g-SiO2 filled coatings was attributed to the good dispersion and distribution of particles. Nano-indention and nano-scratch tests were con- ducted to investigate the scratch resistance of coatings on nano-scale. The surface hardness of the coatings rose by 18% and 14%, and the average friction coefficient decreased by 15% and 11%, respectively, compared to the neat coat due to the addition of 10 wt% g-SiO2 and I-SiO2. The pencil hardness of the coating with 15 wt% g-SiO2 increased from 2B for the neat coating to 2H. However, the pencil hardness of coating with 10 wt% I-SiO2 was only H. The results showed that the g-SiO2 embedded coatings exhibited higher scratch resistance and better optical properties.
基金the financial support provided by National Natural Science Foundation of China (Nos.20821004 and 50642042)the Key Research Program of Ministry ofEducation of China (No. 108009)+1 种基金CNPC Innovation Foundation (No.06-04D-01-01-02)the Chinese Universities Scientific Fund
文摘Pd-based egg-shell nano-catalysts were prepared using porous hollow silica nanoparticles (PHSNs) as support, and the as-prepared catalysts were modified with TiO2 to promote their selectivity for hydro-genation of acetylene. Pd nanoparticles were loaded evenly on PHSNs and TiO2 was loaded on the active Pd particles. The effects of reduction time and temperature and the amount of TiO2 added on catalytic per-formances were investigated by using a fixed-bed micro-reactor. It was found that the catalysts showed better performance when reduced at 300 ℃ than at 500℃, and if reduced for 1 h than 3 h. When the amount of Ti added was 6 times that of Pd, the catalyst showed the highest ethylene selectivity.