Uniform Pd nanoparticles immobilized on N-(3-trimethoxysilylpropyl)diethylenetriamine (PDETA)-functionalized fibrous silica KCC-1 (Pd/KCC-1-PDETA) were prepared with a mean Pd particle size of 2.8 nm. After characteri...Uniform Pd nanoparticles immobilized on N-(3-trimethoxysilylpropyl)diethylenetriamine (PDETA)-functionalized fibrous silica KCC-1 (Pd/KCC-1-PDETA) were prepared with a mean Pd particle size of 2.8 nm. After characterization using powder X-ray diffraction, X-ray photoelectron spectroscopy, and N2 adsorption-desorption isotherms, Pd/KCC-1-PDETA was used as catalyst for additive-free dehydrogenation of formic acid to produce H2. Pd nanoparticle catalysts supported on two other mesoporous silica materials (MSF and KIT-6) were also synthesized to examine how the support affects the reaction. Among the three catalysts, Pd/KCC-1-PDETA exhibited significant catalytic activity (a turnover frequency of 332 h?1 at 323 K and 100% selectivity towards hydrogen), owing to the unique fibrous morphology of KCC-1 and the presence of amine groups that reduced the Pd particle size and improved the access of reactant to the catalytically active Pd sites. The influence of Pd loading (2–10 wt.%), reaction temperature, and reaction time was also examined for the dehydrogenation reaction. Pd/KCC-1-PDETA was recovered easily after the reaction and showed good reusability up to five times without any significant loss in catalytic performance.展开更多
In this research, the influence of several factors such as reaction time, catalyst weight, temperature and different solvents on dehydration reaction of fructose and glucose to 5-hydroxymethylfurfural（HMF） was surve...In this research, the influence of several factors such as reaction time, catalyst weight, temperature and different solvents on dehydration reaction of fructose and glucose to 5-hydroxymethylfurfural（HMF） was surveyed. Nanosphere Al-KCC-1 silica with fibrous morphology was manufactured and used as proficient and recyclable catalyst for this reaction. SEM, TEM, BET, XRD, EDX, elemental mapping, ICP and FT-IR spectroscopy methods were applied for characterization of the Al-KCC-1（molar ratio Si/Al = 5, 40） catalysts. 162℃ and 1 h are the best conditions for the fructose dehydration. Under this situation HMF yield and selectivity are 92.9% and 94.5% respectively and fructose conversion is 98.4%. Also 170℃ and 2 h are the best conditions for the glucose dehydration. In this situation HMF yield and selectivity are 39.0% and39.9% respectively and glucose conversion is 97.8%.展开更多
基金supported by the National Natural Science Foundation of China (220925310, U1162102)the Specialized Research Fund for the Doc-toral of Higher Education (2012007613000)+1 种基金the National Basic Research Program of China (973 Program, 2012BAE05B02)the Shanghai Lead-ing Academic Discipline Project (B409)~~
基金supported by C1 Gas Refinery Program(2015M3D3A1A01064899)by the Ministry of Science,ICT&Future PlanningBasic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education(Grant No.:NRF-2015R1A4A1042434)
文摘Uniform Pd nanoparticles immobilized on N-(3-trimethoxysilylpropyl)diethylenetriamine (PDETA)-functionalized fibrous silica KCC-1 (Pd/KCC-1-PDETA) were prepared with a mean Pd particle size of 2.8 nm. After characterization using powder X-ray diffraction, X-ray photoelectron spectroscopy, and N2 adsorption-desorption isotherms, Pd/KCC-1-PDETA was used as catalyst for additive-free dehydrogenation of formic acid to produce H2. Pd nanoparticle catalysts supported on two other mesoporous silica materials (MSF and KIT-6) were also synthesized to examine how the support affects the reaction. Among the three catalysts, Pd/KCC-1-PDETA exhibited significant catalytic activity (a turnover frequency of 332 h?1 at 323 K and 100% selectivity towards hydrogen), owing to the unique fibrous morphology of KCC-1 and the presence of amine groups that reduced the Pd particle size and improved the access of reactant to the catalytically active Pd sites. The influence of Pd loading (2–10 wt.%), reaction temperature, and reaction time was also examined for the dehydrogenation reaction. Pd/KCC-1-PDETA was recovered easily after the reaction and showed good reusability up to five times without any significant loss in catalytic performance.
基金supported by the Isfahan University of Technology(Iran)
文摘In this research, the influence of several factors such as reaction time, catalyst weight, temperature and different solvents on dehydration reaction of fructose and glucose to 5-hydroxymethylfurfural（HMF） was surveyed. Nanosphere Al-KCC-1 silica with fibrous morphology was manufactured and used as proficient and recyclable catalyst for this reaction. SEM, TEM, BET, XRD, EDX, elemental mapping, ICP and FT-IR spectroscopy methods were applied for characterization of the Al-KCC-1（molar ratio Si/Al = 5, 40） catalysts. 162℃ and 1 h are the best conditions for the fructose dehydration. Under this situation HMF yield and selectivity are 92.9% and 94.5% respectively and fructose conversion is 98.4%. Also 170℃ and 2 h are the best conditions for the glucose dehydration. In this situation HMF yield and selectivity are 39.0% and39.9% respectively and glucose conversion is 97.8%.
