Well-ordered hierarchically mesoporous/microporous carbon materials have been successfully fabricated by using dual soft-templating approach through compressed CO_(2).Pluronic F127 and different type of surfactants,in...Well-ordered hierarchically mesoporous/microporous carbon materials have been successfully fabricated by using dual soft-templating approach through compressed CO_(2).Pluronic F127 and different type of surfactants,including nonionic,cationic,and anionic surfactants,were used as dual templates to investigate the influence on the morphology and nanostructure of the as-prepared carbon samples.TEM,SEM,N2 sorption,wide-angle and small-angle XRD analysis were employed to reveal the well-ordered hierarchically micro-mesoporous structure with2 D hexagonal symmetry by using compressed CO_(2).The prepared HPC samples with different pressures as the catalyst carriers have been functioned by chlorosulfonic acid for the fructose conversion into HMF.Chlorosulfonic acid concentration,catalyst dosage and reaction temperature have been optimized for fructose-to-HMF transformation with the obtained catalyst.The performances of as-made HPC-SO_(3) H samples in HMF yield and reaction rate of fructose-to-HMF transformation have been investigated.The stability of the samples was also conducted in the dehydration of fructose to HMF for five cycles.The possible catalytic mechanism by using hierarchically porous carbon materials as catalyst support for fructose-to-HMF transformation was proposed.展开更多
C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient cat...C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic utilization.Herein,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO clusters.The synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly clarified.These findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.展开更多
基金supported by Beijing Natural Science Foundation (KZ201810028044)。
文摘Well-ordered hierarchically mesoporous/microporous carbon materials have been successfully fabricated by using dual soft-templating approach through compressed CO_(2).Pluronic F127 and different type of surfactants,including nonionic,cationic,and anionic surfactants,were used as dual templates to investigate the influence on the morphology and nanostructure of the as-prepared carbon samples.TEM,SEM,N2 sorption,wide-angle and small-angle XRD analysis were employed to reveal the well-ordered hierarchically micro-mesoporous structure with2 D hexagonal symmetry by using compressed CO_(2).The prepared HPC samples with different pressures as the catalyst carriers have been functioned by chlorosulfonic acid for the fructose conversion into HMF.Chlorosulfonic acid concentration,catalyst dosage and reaction temperature have been optimized for fructose-to-HMF transformation with the obtained catalyst.The performances of as-made HPC-SO_(3) H samples in HMF yield and reaction rate of fructose-to-HMF transformation have been investigated.The stability of the samples was also conducted in the dehydration of fructose to HMF for five cycles.The possible catalytic mechanism by using hierarchically porous carbon materials as catalyst support for fructose-to-HMF transformation was proposed.
基金supported by the National Key Research and Development Program of China(grant no.2022YFA1504901)the National Natural Science Foundation of China(grant nos.22003069,22293012,22179132,22072157,22121002,and 22302209).
文摘C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic utilization.Herein,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO clusters.The synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly clarified.These findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.