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Theoretical design for zeolite synthesis

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Science China Chemistry 2022年第9期65卷 1683-1690页

作者： Qinming Wu Huimin Luan feng-shou xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Key Lab of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 31007China

Zeolites,an important class of microporous crystals,have been widely utilized in the fields of catalysis,ion-exchange,separation,and sorption for a long *** general,zeolites are synthesized in the presence of costly organic templates under hydrothermal conditions by trial-and-error method,which is not only environmentally unfriendly but also *** recent years,novel concepts of design for zeolite synthesis,which are sustainable,cheap,simple,and efficient,have been *** this review,the recent advances in design for zeolite synthesis will be briefly summarized,mainly including the design of organic templates for directing the formation of zeolites,design of organotemplate-free route for zeolite synthesis,design of solvent-free strategy for zeolite synthesis,design for novel interzeolite transformation,and targeted control of zeolite *** review might be helpful for developing sustainable routes for targeted synthesis of zeolites in the future.

关键词： zeolite organic template organotemplate-free solvent-free interzeolite transformation morphology control

New routes for the construction of strong metal-support interactions

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Science China Chemistry 2022年第11期65卷 2051-2057页

作者： Hai Wang Liang Wang feng-shou xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China College of Chemistry Zhengzhou UniversityZhengzhou 450001China

Supported metal nanoparticles(NPs)on solid carriers are highly efficient catalysts in many industrial ***,the sintering and/or leaching of metal NPs occurred under harsh reaction conditions that caused the catalyst *** metal-support interactions(SMSIs)serve as an effective method to stabilize the metal NPs against sintering and leaching,which have been extensively *** addition to the classical route to construct SMSIs via high-temperature reduction treatments,new routes have emerged recently to extend the scope of catalysts with SMSIs and optimized their catalytic *** this review,we briefly summarize these routes that avoid the high-temperature reduction treatments for the construction of *** significant advantages in stabilizing metal NPs,modulating the geometric/electronic structure of metal species,and the mechanism on the SMSI formation are particularly ***,the current challenges and developing trends in the construction of SMSIs for achieving more efficient catalysts are outlooked.

关键词： strong metal-support interaction supported catalyst metal nanoparticles heterogeneous catalysis

Porous Polymeric Catalysts Constructed from Vinylated Functionalities

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Accounts of Materials Research 2022年第7期3卷 772-781页

作者： Qi Sun feng-shou xiao Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

CONSPECTUS:Porous organic polymers(POPs)have revolutionized the production of advanced catalytic materials with unique features such as a large surface area,tunable pore structure,ease of functionalization with a wide range of functional groups,and the ability to function as hosts for encapsulation of functional species,making them appealing for task-specific *** numerous POP-based catalysts have been developed,they are rarely used as a common tool for preparatory-scale operations in laboratories.

关键词： Porous operations Polymeric

Recent Advances in the Synthesis of Zeolites from Solid Wastes

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Chemical Research in Chinese Universities 2024年第4期40卷 646-656页

作者： LIU Pei WU Qinming CHEN Zhenghai xiao feng-shou Key Laboratory of Biomass Chemical Engineering of Ministry of Education and College of Chemical and Biological Engineering Zhejiang UniversityHangzhou310028P.R.China Zhejiang Provincial Innovation Center of Green Petrochemical Technology Ningbo315048P.R.China Kente Catalysts Inc. Xianju317300P.R.China

With the rapid development of industrialization,it is inevitable to produce solid wastes in the fields of energy petrochemical ***,the storage and utilization of these solid wastes have become a considerable *** to the main element composition of these solid wastes including silicon and aluminum,it has attracted extensive attention for synthesizing *** review summarized the properties of major solid wastes including coal fly ash,coal gangue,spent fluid catalytic cracking(FCC)catalyst,lithium slag,bauxite residue,and waste ***,the preparation of LTA,FAU,ZSM-5,SSZ-13,Beta,and MOR zeolites from these solid wastes were ***,the current challenges and perspectives were discussed.

关键词： Solid waste Zeolite Utilization Sustainable route Application

Decorated zeolites for chemoselective alkyne/olefin separations

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Science China Chemistry 2020年第9期63卷 1177-1178页

作者： feng-shou xiao Department of Chemistry Zhejiang UniversityHangzhou 310007China

Light olefins,such as ethylene,propylene,and 1,3-butadiene,are basic chemical raw materials with increasing global demand of approaching 400 million metric tons per *** the industrial production of light olefins,traces of alkyne impurities are co-produced and will show great impacts on the polymerization and subsequent processing of *** purification of olefins is therefore regarded as one of the most important and largest chemical separation processes[1].

关键词： separation approaching propylene

Surprising separation selectivity of ethylene from ethane over pure siliceous zeolites with framework flexibility

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Science China Materials 2018年第5期61卷 763-764页

作者： Xiangju Meng feng-shou xiao Department of Chemistry Zhejiang University

Recovery and purify of light olefins from the off-gas ofthe catalytic crackers have been focused for more than50 years, driven largely by the escalating demand forfeedstock for production of polyethylene and poly-propylene, which requires the separation of C2H4/C2H6and C3H6/C3H8 mixtures in which the olefins and paraf-fins are present at roughly equal concentrations [1,2].

关键词：中国科学材料科学

Silica Modulation of Raney Nickel Catalysts for Selective Hydrogenation

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Precision Chemistry 2023年第5期1卷 309-315页

作者： Yating Lv Hai Wang Huixin Wu Qingsong Luo Liang Wang feng-shou xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

Selective hydrogenation over earth-abundant metal catalysts is challenging but particularly valuable for practical applications in heterogeneous ***,we demonstrate that the catalytic selectivity of the commercial Raney nickel catalyst can be greatly tuned by modulation of the nickel surface by *** quinoline hydrogenation as a model,we show that the silica-modified Raney nickel catalysts exhibit good activity,excellent selectivity,and long stability,whereas the undesired over-hydrogenation reactions are effectively *** contrast,the pristine Raney nickel catalyst shows inferior selectivity for the targeted *** studies confirm a positive role of silica to facilitate the desorption of 1,2,3,4-tetrahydroquinoline from the catalyst surface,thus enhancing the product selectivity.

关键词： selective hydrogenation quinoline 1,2,3,4-tetrahydroquinoline commercial Raney nickel catalyst silica modulation product desorption

CuSx-mediated two reaction systems enable biomimetic photocatalysis in CO_(2) reduction with visible light

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Journal of Energy Chemistry 2022年第2期31卷 497-504页

作者： Ling-Xiang Wang Zhi-Qiang Wang Liang Wang Zhiyuan Yang Qiuyan Zhu Yifeng Liu Wei Fang Xue-Qing Gong Yuefeng Liu xiaolong Liu feng-shou xiao Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310028ZhejiangChina Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Key Laboratory for Advanced Materials and Joint International Research Laboratory for Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterCentre for Computational Chemistry and Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Dalian National Laboratory for Clean Energy(DNL) Dalian Institute of Chemical Physics(DICP)Chinese Academy of ScienceDalian 116023LiaoningChina State Key Laboratory of Optoelectronic Materials and Technologies School of MaterialsSun Yat-Sen UniversityGuangzhou 510275GuangdongChina

The performances of heterogeneous catalysts can be effectively improved by optimizing the catalysts via appropriate structure ***,we show that the catalysis of cuprous sulfide can be boosted by constructing the hybrid structure with Cu_(2)S nanoparticles on amorphous CuSx matrix(Cu_(2)S/CuSx).In the photocatalytic CO_(2) reduction under visible light irradiation,the Cu_(2)S/CuSx exhibited a CO production rate at 4.0μmol h-1 that is 12-fold higher than that of the general Cu_(2)S *** characterizations reveal that the Cu_(2)S/CuSx has two reaction systems that realize the biomimetic catalysis,involving in the light reaction on the Cu_(2)S nanoparticle-CuSx matrix heterojunctions for proton/electron production,and the dark reaction on the defect-rich CuSx for CO_(2) *** CuSx matrix could efficiently activate CO_(2) and stabilize the split hydrogen species to hinder undesired hydrogen evolution reaction,which benefits the proton-electron transfer to reduce CO_(2),a key step for bridging the two reaction systems.

关键词： CO_(2) Photoreduction Bifunctional catalyst Proton-coupled electron transfer

调控铝在ITH沸石骨架中的位置以用于催化甲醇制烯烃

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Chinese Journal of Catalysis 2024年第1期56卷 114-121页

作者：范凯吴勤明刘烁孔海宇王森 Eduard Kunkes Trees De Baerdemaeker Andrei-Nicolae Parvulescu Nils Bottke Toshiyuki Yokoi Dirk E.De Vos 孟祥举张维萍肖丰收浙江省应用化学重点实验室浙江大学化学系中国浙江杭州310028 浙江大学化学与生物工程学院中国浙江杭州310028 大连理工大学精细化工国家重点实验室中国辽宁大连116012 中国科学院山西煤炭化学研究所煤转化国家重点实验室中国山西太原030001 巴斯夫股份有限公司德国东京工业大学资源化学研究所日本鲁汶大学表面化学与催化中心比利时

随着低碳烯烃需求量的增加,甲醇制烯烃(MTO)成为由非石油资源制取低碳烯烃的关键技术,其中沸石由于具有可调节的酸度、有序的微孔结构和较好的择型性能而被广泛用作MTO反应催化剂.ITQ-13沸石(ITH拓扑结构)由于其独特的九元环结构在MTO... 详细信息

随着低碳烯烃需求量的增加,甲醇制烯烃(MTO)成为由非石油资源制取低碳烯烃的关键技术,其中沸石由于具有可调节的酸度、有序的微孔结构和较好的择型性能而被广泛用作MTO反应催化剂.ITQ-13沸石(ITH拓扑结构)由于其独特的九元环结构在MTO反应中表现出较好的丙烯选择性和反应寿命,引起了广泛关注.研究表明,分子筛的酸中心分布与MTO反应性能密切相关,因此,研究ITQ-13沸石中铝分布与MTO反应性能的关系,对进一步提升其MTO催化性能具有重要意义.本文分别以与ITH具有共同基本结构单元(双四元环,D4Rs)的LTA沸石(LTA-ITH)和薄水铝石(C-ITH)为铝源,合成了两类铝硅酸盐ITH沸石.X射线衍射、扫描电子显微镜以及氮气吸脱附表征结果表明,这两类分子筛具有相似的片状形貌和微孔性质.氨气程序升温脱附结果表明,具有相近硅铝比的两类ITH沸石具有相近的酸量.进一步采用27Al魔角旋转核磁共振(MAS NMR)、密度泛函理论计算和1-己烯裂解反应对两类ITH分子筛的铝分布进行研究.结果表明,两类分子筛具有不同的铝分布,LTA-ITH中有更多的铝进入ITH的正弦孔道与直孔道,而C-ITH中有更多的铝分布在交叉孔道.当前,研究者普遍认为MTO反应过程遵循双循环烃池机理,ITH交叉孔道由于具有较大的空间,相比于正弦孔道和直孔道,更有利于芳烃循环中间体的产生,从而有利于形成芳烃循环产物(乙烯),而正弦孔道和直孔道却更有利于烯烃循环过程,导致产生更多的丙烯.对两类ITH进行了MTO催化性能测试,结果表明,LTA-ITH比C-ITH表现出更高的丙烯选择性,并且表现出更高的丙烯与乙烯的比率,表明其烯烃循环过程得到加强,这与^(27)Al MAS NMR以及1-己烯裂解反应得到的结论一致,进一步证明ITH分子筛的铝分布得到有效调控.综上,本文阐明了ITH沸石中铝分布与其反应性能的关系,为调整沸石骨架中的Al位点提供一种新策略,为未来制备高效的MTO沸石基催化剂提供参考.

关键词：骨架铝分布硅铝ITH分子筛甲醇制烯烃铝核磁