Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficien...Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.展开更多
The adsorb model of formic acid on NaX derived from TPD was discussed. It was showed that the adsorb sites were various exposed framework O2- centers bearing different basic intensity and spatial resistance. The h-pea...The adsorb model of formic acid on NaX derived from TPD was discussed. It was showed that the adsorb sites were various exposed framework O2- centers bearing different basic intensity and spatial resistance. The h-peak was attributed to O2- near S-III in supercage and l-peak to O2- near S-II in beta-cage of faujusite zeolite. The model can explain the experimental results. Meanwhile, a relative standard of basic intensity based on TPD of formic acid was founded.展开更多
In this paper the effect of ion-exchange simplified as water handling on basic zeolitewas studied.It was foond that the interaction between chemisorbed water and Na+-O2- couplewould increase the total number of basic ...In this paper the effect of ion-exchange simplified as water handling on basic zeolitewas studied.It was foond that the interaction between chemisorbed water and Na+-O2- couplewould increase the total number of basic sites, while weaken the intensity of each basic sites.Theprocess can be explained by the adsorb model of organic acid on NaX presented before.展开更多
基金The financial supports from the National Natural Science Foundation of China (22178059, 22208054 and 22072019)Natural Science Foundation of Fujian Province, China (2020J01513)+1 种基金Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS0076)Qingyuan Innovation Laboratory (00121002)
文摘Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.
文摘The adsorb model of formic acid on NaX derived from TPD was discussed. It was showed that the adsorb sites were various exposed framework O2- centers bearing different basic intensity and spatial resistance. The h-peak was attributed to O2- near S-III in supercage and l-peak to O2- near S-II in beta-cage of faujusite zeolite. The model can explain the experimental results. Meanwhile, a relative standard of basic intensity based on TPD of formic acid was founded.
文摘In this paper the effect of ion-exchange simplified as water handling on basic zeolitewas studied.It was foond that the interaction between chemisorbed water and Na+-O2- couplewould increase the total number of basic sites, while weaken the intensity of each basic sites.Theprocess can be explained by the adsorb model of organic acid on NaX presented before.
