, Abstract ： The S A P O - 5 and S n S A P O - 5 molecular sieves were successfully prepared by directly adding Si and Sn'+ sources into the gel. The physical and chemical jiroperties of molecular sieves were investigated by XRI), low tem perature N : physical adsorption, S E M , N M R , Py-IR and With the increase of Sn content, the crrstal surface of S n S A P O - 5 is smoother and the appearance is more regular hexagonal prisms. The Sn and Si are more con-cenlrated on the surface of molecular sieves. In addition, the framework Al is replaced by Sn 2+, causing defects in the framework, im!)alance of cliarges and more acidic sites. The molecular sieves were used to modify tlie N i W cata lyst, and dihenzotliiophene ( D B T ) in the simulated oil was used as a prol)e to evaluate the H D S performance of their modified hydrogenation catalysts. The addition of S n S A P O - 5 in the catalyst introduces more acidic* sites, im proves the interaction between support and active metals, promotes the suliidation of active metals, and forms more metal active phases, thereby the hydrodesulfurization capacity of the N i W catalyst was improved. Therefore, the catalyst modified by S n S A P O - 5 has better H D S activity than other catalysts, and has better application prospect.
{"title":"Research on Properties of Sn and Si Doped AlPO4-5 Molecular Sieve and Its Hydrodesulfurization Reaction","authors":"化冰 张, 厚祥 孙","doi":"10.3724/SP.J.7103291365","DOIUrl":"https://doi.org/10.3724/SP.J.7103291365","url":null,"abstract":", Abstract ： The S A P O - 5 and S n S A P O - 5 molecular sieves were successfully prepared by directly adding Si and Sn'+ sources into the gel. The physical and chemical jiroperties of molecular sieves were investigated by XRI), low tem perature N : physical adsorption, S E M , N M R , Py-IR and With the increase of Sn content, the crrstal surface of S n S A P O - 5 is smoother and the appearance is more regular hexagonal prisms. The Sn and Si are more con-cenlrated on the surface of molecular sieves. In addition, the framework Al is replaced by Sn 2+, causing defects in the framework, im!)alance of cliarges and more acidic sites. The molecular sieves were used to modify tlie N i W cata lyst, and dihenzotliiophene ( D B T ) in the simulated oil was used as a prol)e to evaluate the H D S performance of their modified hydrogenation catalysts. The addition of S n S A P O - 5 in the catalyst introduces more acidic* sites, im proves the interaction between support and active metals, promotes the suliidation of active metals, and forms more metal active phases, thereby the hydrodesulfurization capacity of the N i W catalyst was improved. Therefore, the catalyst modified by S n S A P O - 5 has better H D S activity than other catalysts, and has better application prospect.","PeriodicalId":412338,"journal":{"name":"Journal of Molecular Catalysis(China)","volume":"8 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2020-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"123888182","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
： The effects of mechanical stirring, ingredient composition and ciystallization parameters on hvclrothermal synthesis of S A P O - 3 4 and S A P O - 5 silicoaluminophosphate zeolites were investigated. The effects of granule-mixing process and powder-grinding process on the preparation of "silicoaluminophosphate zeolite/spiner' composite cata lysts were investigated. Compared with S A P O - 3 4 zeolite, S A P O - 5 zeolite ciystals exhibited stronger tolerance to m e chanical action. X R D , physical adsorption, F E S E M and E D S were em])loyed to investigate the structure and tex-ture features of the materials. The catalytic performance of four composite catalysts for C O hydrogenation was c o m pared. The sequence of phases which can make a composite catalyst more suppress C —— C coupling and produce more light hydrocaibons is ： S A P O - 3 4 > S A P O - 5 > tlZ n A l C ^ 0 4，， spinel phase. The sequence of phases that can mak e a composite catalyst have higher C O hydrogenation activity ( i.e., C O conversion) is: “ZnAlCi.04” spinel phase > S A P O - 3 4
考察了机械搅拌、原料组成和结晶参数对湿热合成硫酸磷- 34和硫酸磷- 5硅铝磷酸盐分子筛的影响。研究了混粒工艺和粉磨工艺对制备“硅铝磷沸石/纺丝”复合催化剂的影响。与硫酸磷- 34分子筛相比，硫酸磷- 5分子筛具有更强的力学耐受力。采用X - R - D、物理吸附、fe - S - E - M和E - D - S等方法研究了材料的结构和织构特征。比较了四种复合催化剂对一氧化碳加氢的催化性能。复合催化剂中抑制C—C偶联和生成轻烃的相序为:s&a P O - 34 > s&a P O - 5 > tlZ n al C ^ 0 4，尖晶石相。能使复合催化剂具有较高的一氧化碳加氢活性(即一氧化碳转化)的相顺序为:“ZnAlCi”。4”尖晶石相> S A P O - 3
{"title":"Crystallization of SAPO Series Silicoaluminophosphate Zeolites and Effect of Their Composite Catalysts on CO Hydrogenation","authors":"贾 高鹏, 高 玉集, 赵 晨曦, 田 红美, 刘 振新","doi":"10.3724/SP.J.7103291364","DOIUrl":"https://doi.org/10.3724/SP.J.7103291364","url":null,"abstract":"： The effects of mechanical stirring, ingredient composition and ciystallization parameters on hvclrothermal synthesis of S A P O - 3 4 and S A P O - 5 silicoaluminophosphate zeolites were investigated. The effects of granule-mixing process and powder-grinding process on the preparation of \"silicoaluminophosphate zeolite/spiner' composite cata lysts were investigated. Compared with S A P O - 3 4 zeolite, S A P O - 5 zeolite ciystals exhibited stronger tolerance to m e chanical action. X R D , physical adsorption, F E S E M and E D S were em])loyed to investigate the structure and tex-ture features of the materials. The catalytic performance of four composite catalysts for C O hydrogenation was c o m pared. The sequence of phases which can make a composite catalyst more suppress C —— C coupling and produce more light hydrocaibons is ： S A P O - 3 4 > S A P O - 5 > tlZ n A l C ^ 0 4，， spinel phase. The sequence of phases that can mak e a composite catalyst have higher C O hydrogenation activity ( i.e., C O conversion) is: “ZnAlCi.04” spinel phase > S A P O - 3 4","PeriodicalId":412338,"journal":{"name":"Journal of Molecular Catalysis(China)","volume":"24 2 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2020-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"121323396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
： The manganese oxide octahedral molecular sieve ( O M S -2) , because of its excellent oxidation , adsorp tion , ion - exchange , and conductivity properties , was wildly used in various fields such as environmental , semicon ductor , synthetic organic . Because of the mixed valency in the framework and abundant surface defect vacancy , O M S -2 could effectively activate green oxidants such as oxygen and hydrogen peroxide , making it an effective heter ogeneous catalyst and functional supporterin clean synthesis of organic molecules . Moreover , the O M S -2 catalysis material exhiliited excellent activity , selectivity , and structural stability . W e reviewed O M S -2 as heterogeneous cat alyst and electron transfer medium (also as functional supporter in supported catalysts ) in the clean oxidation syn thesis of organic molecules . Finally , the existing problems and future development of O M S -2 -catalyzed oxidations were
氧化锰八面体分子筛(O M S -2)由于其优异的氧化、吸附、离子交换和导电性能，在环境、半导体、有机合成等领域得到了广泛的应用。由于O M S -2骨架内的混合价态和丰富的表面缺陷空位，可以有效激活氧和过氧化氢等绿色氧化剂，成为清洁合成有机分子的有效异相催化剂和功能载体。此外，O M S -2催化材料表现出优异的活性、选择性和结构稳定性。本文综述了oms2作为非均相催化剂和电子传递介质(也可作为负载型催化剂的功能载体)在有机分子清洁氧化合成中的应用。最后，对O - M - S -2催化氧化存在的问题及今后的发展方向进行了展望
{"title":"Application of Manganese Oxide Octahedral Molecular Sieves(OMS-2)in Clean Synthesis of Organic Compounds","authors":"赵 培庆, 毕 秀茹","doi":"10.3724/SP.J.7103291367","DOIUrl":"https://doi.org/10.3724/SP.J.7103291367","url":null,"abstract":"： The manganese oxide octahedral molecular sieve ( O M S -2) , because of its excellent oxidation , adsorp tion , ion - exchange , and conductivity properties , was wildly used in various fields such as environmental , semicon ductor , synthetic organic . Because of the mixed valency in the framework and abundant surface defect vacancy , O M S -2 could effectively activate green oxidants such as oxygen and hydrogen peroxide , making it an effective heter ogeneous catalyst and functional supporterin clean synthesis of organic molecules . Moreover , the O M S -2 catalysis material exhiliited excellent activity , selectivity , and structural stability . W e reviewed O M S -2 as heterogeneous cat alyst and electron transfer medium (also as functional supporter in supported catalysts ) in the clean oxidation syn thesis of organic molecules . Finally , the existing problems and future development of O M S -2 -catalyzed oxidations were","PeriodicalId":412338,"journal":{"name":"Journal of Molecular Catalysis(China)","volume":"4 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2020-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"124272955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
： Tungsten carbide has attracted extensive attention in the field of electrocatalytic hydrogen evolution due to its uni(|ue Pt like electronic structure and catalytic performance. He*teroatom doping and the constmction of nano materials with high specific suiface area are important strategies to further improve their propeilies. In this study, the heteroatom doped tungsten carbide with high specific surface area was prepared by controlled carbonization of u-rea formaldehyde resin with rich polar func tional groups as the substrate and polyoxonietalate clusters uniformly sup ported on its branched chain skeleton ( P - W - , C @ N C ) all j)H hydrogen evolution catalyst. The B K T specific surface area of the material is 136 • g _l. X R D , X P S , S E M and T E M results show that the catalyst is composed of tung sten carbide nanoparticles with phosphorus eloping and a thin nitrogen doped carbon layer coated oil the surface of tungsten carl)ide particles. In 0.5 mol/L sulfuric acid, 1 mol/L potassium hydroxide and 0.1 niol/L sulfuric acid buffer solution, the current density of 10 m A • c m " 2 can I)e achieved only by over potential of 83, 63 and 179 m V respectively, and this catalyst have long-term catalytic stability.
碳化钨由于具有类似铂的单一电子结构和催化性能，在电催化析氢领域引起了广泛的关注。杂原子掺杂和构建具有高比表面积的纳米材料是进一步提高其性能的重要策略。本研究以富极性官能团的脲醛树脂为底物，在支链骨架(P - W -， C @ N C)全j)H催化剂上均匀支撑聚氧乙酸酯簇，通过可控碳化法制备了具有高比表面积的杂原子掺杂碳化钨。材料的bkt比表面积为136•g_l。X R D、X P S、S E M和T E M结果表明，该催化剂由含磷的碳化钨纳米颗粒和包覆在碳化钨颗粒表面的薄氮掺杂碳层组成。在0.5 mol/L硫酸、1 mol/L氢氧化钾和0.1 niol/L硫酸缓冲溶液中，仅在超过电位分别为83、63和179 m V时，即可达到10 m A•c m“2”的电流密度，且该催化剂具有长期的催化稳定性。
{"title":"Urea-formaldehyde Resin Derived P-doped Tungsten Carbide on N-carbon Sheets(P-W2C@NC)as All pH HER Catalyst","authors":"韩 苗苗","doi":"10.3724/SP.J.7103291366","DOIUrl":"https://doi.org/10.3724/SP.J.7103291366","url":null,"abstract":"： Tungsten carbide has attracted extensive attention in the field of electrocatalytic hydrogen evolution due to its uni(|ue Pt like electronic structure and catalytic performance. He*teroatom doping and the constmction of nano materials with high specific suiface area are important strategies to further improve their propeilies. In this study, the heteroatom doped tungsten carbide with high specific surface area was prepared by controlled carbonization of u-rea formaldehyde resin with rich polar func tional groups as the substrate and polyoxonietalate clusters uniformly sup ported on its branched chain skeleton ( P - W - , C @ N C ) all j)H hydrogen evolution catalyst. The B K T specific surface area of the material is 136 • g _l. X R D , X P S , S E M and T E M results show that the catalyst is composed of tung sten carbide nanoparticles with phosphorus eloping and a thin nitrogen doped carbon layer coated oil the surface of tungsten carl)ide particles. In 0.5 mol/L sulfuric acid, 1 mol/L potassium hydroxide and 0.1 niol/L sulfuric acid buffer solution, the current density of 10 m A • c m \" 2 can I)e achieved only by over potential of 83, 63 and 179 m V respectively, and this catalyst have long-term catalytic stability.","PeriodicalId":412338,"journal":{"name":"Journal of Molecular Catalysis(China)","volume":"42 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2020-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"125588989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
： With the shortage of fossil fuels and the environmental problems caused by their utilization, renewable biomass resources have gradually become an important source for the production of fuel and chemicals. In recent years, as the main by-product of biodiesel production, glycerol has attracted widespread attention. The utilization of glycerol to produce high value-added products and the development of relevant conversion technologies have also be come a hot spot for scholars at h o m e and abroad. A m o n g m a n y conversion technologies, the selective oxidation of glycerin to acrylic acid has shown broad development prospects. It has important economic and social significance to study the reaction and especially the catalyst. This article summarizes the current research status of composite metal oxide catalysts for the selective oxidation of glycerol to aciylic acid. The cuiTent types of catalytic systems used in the reaction and the understanding of the catalytic reaction mechanism of glycerol oxidation to aciylic acid are brief ly introduced. Moreover, the existing problems and future prospects are also analyzed and expected.
{"title":"Research Progress of Composite Metal Oxide Catalysts for the Oxidation of Glycerol to Acrylic Acid","authors":"三三 于, 自轩 卢, 双明 李","doi":"10.3724/SP.J.7103291369","DOIUrl":"https://doi.org/10.3724/SP.J.7103291369","url":null,"abstract":"： With the shortage of fossil fuels and the environmental problems caused by their utilization, renewable biomass resources have gradually become an important source for the production of fuel and chemicals. In recent years, as the main by-product of biodiesel production, glycerol has attracted widespread attention. The utilization of glycerol to produce high value-added products and the development of relevant conversion technologies have also be come a hot spot for scholars at h o m e and abroad. A m o n g m a n y conversion technologies, the selective oxidation of glycerin to acrylic acid has shown broad development prospects. It has important economic and social significance to study the reaction and especially the catalyst. This article summarizes the current research status of composite metal oxide catalysts for the selective oxidation of glycerol to aciylic acid. The cuiTent types of catalytic systems used in the reaction and the understanding of the catalytic reaction mechanism of glycerol oxidation to aciylic acid are brief ly introduced. Moreover, the existing problems and future prospects are also analyzed and expected.","PeriodicalId":412338,"journal":{"name":"Journal of Molecular Catalysis(China)","volume":"3 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2020-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"131334206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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