Ceramic ultrafiltration membranes were used to separate titanium silicalite-1 (TS-1) catalysts from the slurry of catalytic ammoximation of cyclohexanone to oxime. Silica was shown to have a great effect on membrane...Ceramic ultrafiltration membranes were used to separate titanium silicalite-1 (TS-1) catalysts from the slurry of catalytic ammoximation of cyclohexanone to oxime. Silica was shown to have a great effect on membrane fouling in the alkaline environment of this system. In the ammoximation system, there are three main silica sources, which are residual silica on the catalyst particles surface during preparation, silica dissolved from TS-1 catalyst particles by ammonia solvent, and silica sol added into the reaction slurry to inhibit the dissolution erosion of the TS-1 catalyst. The silica dissolved by ammonia has been proved to influence membrane fouling most among the three silica sources. This was because the amount of silica dissolved by ammonia was the largest, and the polymerization of silica monomers at high concentration caused colloid particles formation, which led to a dense cake layer depositing on the membrane surface. Meanwhile, the size reduction of catalyst particles caused by alkaline dissolution also increased specific resistances of cake layers.展开更多
Tailoring the Ti coordination states in titanosilicate zeolites to simultaneously improve feedstock conversion and maximize the target product selectivity remains a challenge in the pursuit of high-performance catalys...Tailoring the Ti coordination states in titanosilicate zeolites to simultaneously improve feedstock conversion and maximize the target product selectivity remains a challenge in the pursuit of high-performance catalysts for selective oxidation reactions.Herein,we provide a facile strategy to synthesize hierarchical anatase-free TS-1(MFI-type)zeolites with tetrahedrally coordinated(TiO_(4))and octahedrally coordinated Ti species(TiO_(6)).The TiO_(4)species provide high epoxide selectivity,while the TiO_(6)species afford improved alkene conversion.This strategy is achieved by synergistically using an L-lysine-assisted approach and a two-step crystallization;the two-step crystallization approach prevents the formation of anatase TiO_(2),while L-lysine stabilizes the TiO_(6)species and ensures efficient incorporation of TiO_(6)into the anatase-free TS-1 zeolites.Compared with their conventional counterparts,which only contain TiO_(4)species,the as-prepared TS-1 zeolites(Si/Ti=36.9)result in a higher 1-hexene conversion(33%),higher TON value(153),and comparable epoxide selectivity(95%).This synthetic strategy provides avenues to tailor the amount and distribution of Ti species in titanosilicate zeolites to achieve high catalytic performances in various processes.展开更多
The epoxidation reaction of propylene and hydrogen peroxide with zeolite catalyst containing titaniumsilicalite (TS-1)has been studied, and the reaction in the mixed solvent of water/methanol has been discussed. It is...The epoxidation reaction of propylene and hydrogen peroxide with zeolite catalyst containing titaniumsilicalite (TS-1)has been studied, and the reaction in the mixed solvent of water/methanol has been discussed. It is shown that the selective of epoxidation propylene decreases while the selective of propylene glycol increases, when the water content increases in the mixed solvent of methanol/water.展开更多
Let MPT ( v,λ ) denote a maximum packing of triples of order v with index λ and TS ( u,λ ) denote a triple system of order u with index λ . In this paper, for v ≥6, we determine necessary and sufficient condition...Let MPT ( v,λ ) denote a maximum packing of triples of order v with index λ and TS ( u,λ ) denote a triple system of order u with index λ . In this paper, for v ≥6, we determine necessary and sufficient conditions for enclosing an MPT ( v,λ ) in a TS ( v+1,λ+m ) with one extra point and minimal increase in λ .展开更多
基金Supported by the National Basic Research Program of China (2009CB623406), the National Natural Science Foundation of China (20806038), the Natural Science Foundation of Jiangsu Province (BK2008504), the National Science Foundation for Postdoctoral Scientists of China (20070421005) and Jiangsu Planned Projects for Postdoctoral Research Funds (0702020B).
文摘Ceramic ultrafiltration membranes were used to separate titanium silicalite-1 (TS-1) catalysts from the slurry of catalytic ammoximation of cyclohexanone to oxime. Silica was shown to have a great effect on membrane fouling in the alkaline environment of this system. In the ammoximation system, there are three main silica sources, which are residual silica on the catalyst particles surface during preparation, silica dissolved from TS-1 catalyst particles by ammonia solvent, and silica sol added into the reaction slurry to inhibit the dissolution erosion of the TS-1 catalyst. The silica dissolved by ammonia has been proved to influence membrane fouling most among the three silica sources. This was because the amount of silica dissolved by ammonia was the largest, and the polymerization of silica monomers at high concentration caused colloid particles formation, which led to a dense cake layer depositing on the membrane surface. Meanwhile, the size reduction of catalyst particles caused by alkaline dissolution also increased specific resistances of cake layers.
文摘Tailoring the Ti coordination states in titanosilicate zeolites to simultaneously improve feedstock conversion and maximize the target product selectivity remains a challenge in the pursuit of high-performance catalysts for selective oxidation reactions.Herein,we provide a facile strategy to synthesize hierarchical anatase-free TS-1(MFI-type)zeolites with tetrahedrally coordinated(TiO_(4))and octahedrally coordinated Ti species(TiO_(6)).The TiO_(4)species provide high epoxide selectivity,while the TiO_(6)species afford improved alkene conversion.This strategy is achieved by synergistically using an L-lysine-assisted approach and a two-step crystallization;the two-step crystallization approach prevents the formation of anatase TiO_(2),while L-lysine stabilizes the TiO_(6)species and ensures efficient incorporation of TiO_(6)into the anatase-free TS-1 zeolites.Compared with their conventional counterparts,which only contain TiO_(4)species,the as-prepared TS-1 zeolites(Si/Ti=36.9)result in a higher 1-hexene conversion(33%),higher TON value(153),and comparable epoxide selectivity(95%).This synthetic strategy provides avenues to tailor the amount and distribution of Ti species in titanosilicate zeolites to achieve high catalytic performances in various processes.
文摘The epoxidation reaction of propylene and hydrogen peroxide with zeolite catalyst containing titaniumsilicalite (TS-1)has been studied, and the reaction in the mixed solvent of water/methanol has been discussed. It is shown that the selective of epoxidation propylene decreases while the selective of propylene glycol increases, when the water content increases in the mixed solvent of methanol/water.
文摘Let MPT ( v,λ ) denote a maximum packing of triples of order v with index λ and TS ( u,λ ) denote a triple system of order u with index λ . In this paper, for v ≥6, we determine necessary and sufficient conditions for enclosing an MPT ( v,λ ) in a TS ( v+1,λ+m ) with one extra point and minimal increase in λ .