SSZ-13和SAPO-34是性能优异的甲醇制烯烃(methanol to olefins,MTO)催化剂。本文从酸性、积炭、烃池物种及其反应途径等方面介绍了SSZ-13和SAPO-34的酸强度和酸中心密度的差异及其对MTO反应催化性能的影响,综述了SSZ-13和SAPO-34在MTO...SSZ-13和SAPO-34是性能优异的甲醇制烯烃(methanol to olefins,MTO)催化剂。本文从酸性、积炭、烃池物种及其反应途径等方面介绍了SSZ-13和SAPO-34的酸强度和酸中心密度的差异及其对MTO反应催化性能的影响,综述了SSZ-13和SAPO-34在MTO中的催化反应机理和失活机理的研究进展。总结显示,尽管SSZ-13和SAPO-34都是CHA型拓扑结构,但SSZ-13的酸性强于SAPO-34,更有利于碳正离子的生成;与修边机理相比,侧链烷基化机理是更主要的反应途径,且SSZ-13的甲基化速率比SAPO-34高3个数量级;SSZ-13和SAPO-34的积炭速率和积炭物种存在差异,积炭行为受温度影响较大。从催化剂的角度,指出合理调控酸强度和酸中心密度、研制出能够抑制反应失活的催化剂结构、发展高产乙烯或者丙烯的特色MTO催化剂是以后的研究方向;从反应机理的角度,认为SSZ-13和SAPO-34在MTO反应中活性中间体的形成以及转化途径、活性物种到积炭物种的演变有待进一步研究。此外,如何在MTO反应过程中观察到高活性的反应中间体是今后研究的难点。展开更多
Using coal gangue(CG)as raw material,a new type of all solid-waste-based 13-X molecular sieve material was controllably prepared by alkali fusion-hydrothermal method.The synthetic molecular sieve was used as a solid a...Using coal gangue(CG)as raw material,a new type of all solid-waste-based 13-X molecular sieve material was controllably prepared by alkali fusion-hydrothermal method.The synthetic molecular sieve was used as a solid adsorbent to treat Cd^(2+)-containing wastewater,and its adsorption behavior on Cd^(2+)in aqueous solution was studied and analyzed.The microstructure and morphology of the molecular sieve were investigated by X-ray diffraction(XRD),field emission scanning electron microscopy(FESEM)and specific surface area analyzer.The results show that the synthesized 13-X molecular sieve has higher Brunauer–Emmett–Teller(BET)specific surface area with higher crystallinity and higher adsorption capacity for the heavy metal Cd^(2+).The adsorption process of Cd^(2+)by molecular sieve conforms to the Langmuir isotherm adsorption equation and Lagergren pseudo-second-order rate equation.Combined with thermodynamic calculation,it can be concluded that the adsorption process is physically monolayer,spontaneous and exothermic.In this study,a low-cost and naturally available synthesis method of 13-X molecular sieve is reported.Combined with its adsorption mechanism for Cd^(2+),it provides a feasible and general method for removing heavy metal ions from coal gangue and also provides a new way for the utilization of coal gangue with high added value.展开更多
文摘SSZ-13和SAPO-34是性能优异的甲醇制烯烃(methanol to olefins,MTO)催化剂。本文从酸性、积炭、烃池物种及其反应途径等方面介绍了SSZ-13和SAPO-34的酸强度和酸中心密度的差异及其对MTO反应催化性能的影响,综述了SSZ-13和SAPO-34在MTO中的催化反应机理和失活机理的研究进展。总结显示,尽管SSZ-13和SAPO-34都是CHA型拓扑结构,但SSZ-13的酸性强于SAPO-34,更有利于碳正离子的生成;与修边机理相比,侧链烷基化机理是更主要的反应途径,且SSZ-13的甲基化速率比SAPO-34高3个数量级;SSZ-13和SAPO-34的积炭速率和积炭物种存在差异,积炭行为受温度影响较大。从催化剂的角度,指出合理调控酸强度和酸中心密度、研制出能够抑制反应失活的催化剂结构、发展高产乙烯或者丙烯的特色MTO催化剂是以后的研究方向;从反应机理的角度,认为SSZ-13和SAPO-34在MTO反应中活性中间体的形成以及转化途径、活性物种到积炭物种的演变有待进一步研究。此外,如何在MTO反应过程中观察到高活性的反应中间体是今后研究的难点。
文摘以硅溶胶、硫酸铝、氢氧化钠、去离子水为原料,以N,N,N-三甲基金钢烷氢氧化铵为模板剂(R),用传统的水热法合成分子筛SSZ-13,对合成产物用XRD、SEM、FT-IR和BET进行表征,并通过改变原料的配比和反应条件确定它的最佳合成条件.实验结果表明:在反应温度为155℃、晶化时间为3 d时,其最佳合成氧化物的摩尔比范围:SiO2/A12O3为40,Na2O/A12O3为12～16,R2O/A12O3为3～5,H2O/A12O3为900～1 350.在最佳条件下合成的分子筛SSZ-13,大大缩短了反应时间,加晶种或促进剂时,晶化时间缩短为2 d.
基金This study was financially supported by the National Natural Science Foundation of China(No.52172099)the Basic Research Plan of Natural Science of Shaanxi Province(No.2020JQ-754)+3 种基金the Key Innovation Team of Shaanxi Province(No.2014KCT-04)the Excellent Youth Science and Technology Fund Project of Xi'an University of Science and Technology(Grant No.6310221009)the Excellent Youth Science and Technology Fund Project of Xi'an University of Science and Technology(Grant No.6310221009)the Special Project of Shaanxi Province(No.19JK0490)and the Study on Preparation and Properties of New Solid-Wastebased Cementitious Materials(No.6000190120).
文摘Using coal gangue(CG)as raw material,a new type of all solid-waste-based 13-X molecular sieve material was controllably prepared by alkali fusion-hydrothermal method.The synthetic molecular sieve was used as a solid adsorbent to treat Cd^(2+)-containing wastewater,and its adsorption behavior on Cd^(2+)in aqueous solution was studied and analyzed.The microstructure and morphology of the molecular sieve were investigated by X-ray diffraction(XRD),field emission scanning electron microscopy(FESEM)and specific surface area analyzer.The results show that the synthesized 13-X molecular sieve has higher Brunauer–Emmett–Teller(BET)specific surface area with higher crystallinity and higher adsorption capacity for the heavy metal Cd^(2+).The adsorption process of Cd^(2+)by molecular sieve conforms to the Langmuir isotherm adsorption equation and Lagergren pseudo-second-order rate equation.Combined with thermodynamic calculation,it can be concluded that the adsorption process is physically monolayer,spontaneous and exothermic.In this study,a low-cost and naturally available synthesis method of 13-X molecular sieve is reported.Combined with its adsorption mechanism for Cd^(2+),it provides a feasible and general method for removing heavy metal ions from coal gangue and also provides a new way for the utilization of coal gangue with high added value.
