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Enhanced aromatic selectivity by the sheet-like ZSM-5 in syngas conversion

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Journal of Energy Chemistry 2019年第8期28卷 44-48,I0003页

作者： Junhao Yang Ke Gong Dengyun Miao Feng Jiao Xiulian Pan Xiangju Meng fengshou xiao Xinhe Bao State Key Laboratory of Catalysis National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of SciencesZhongshan Road 457 Dalian 116023 Liaoning China University of Chinese Academy of Sciences Yuquan Road 19A Shijingshan District Beijing 100049 China Department of Chemistry Zhejiang UniversityTianmushan Road 148 Xihu District Hangzhou 310028 Zhejiang China

Aromatics are important basic chemicals. However, direct conversion of syngas via the conventional Fischer-Tropsch synthesis produces little aromatics. We presented herein that a bifunctional composite of ZSM-5 in combination with Zn Cr Oxcatalyzes syngas conversion to aromatics. Particularly, ZSM-5 crystals with a sheet-like morphology can enhance significantly the aromatization activity. The lower length ratio of the b/a axes of the crystals, the more aromatics form but without influencing the selectivity of small molecules such as CH4 and C2–C4. Since the acid properties and the Al chemical environment were not altered while the morphology changed, the enhanced aromatic selectivity is likely attributed to the favored diffusion of aromatics in these sheet-like crystals.

关键词： Synthesis gas Aromatics Bifunctional OX-ZEO catalyst Zeolite Morphology

Theoretical design for zeolite synthesis

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Science China Chemistry 2022年

作者： Qinming Wu Huimin Luan fengshou xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Key Lab of Applied Chemistry of Zhejiang Province Department of Chemistry Zhejiang University

Zeolites, an important class of microporous crystals, have been widely utilized in the fields of catalysis, ion-exchange, separation, and sorption for a long time. In 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 labor-intensive. In recent years, novel concepts of design for zeolite synthesis, which are sustainable, cheap, simple, and efficient, have been developed. In 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 morphologies. This review might be helpful for developing sustainable routes for targeted synthesis of zeolites in the future.

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Organosilane surfactant-assisted synthesis of mesoporous SSZ-39 zeolite with enhanced catalytic performance in the methanol-to-olefins reaction

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Frontiers of Chemical Science and Engineering 2020年第2期14卷 267-274页

作者： Hao Xu Chi Lei Qinming Wu Qiuyan Zhu Xiangju Meng Daniel Dai Stefan Maurer Andrei-Nicolae Parvulescu Ulrich Muller fengshou xiao Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310028China BASF Catalysts(Shanghai)Co. Ltd.Shanghai 201206China BASF SE Ludwigshafen 67056Germany

SSZ-39 zeolite with AEI framework structure is a good catalyst candidate for the methanol-to-olefins(MTO)***,the diffusion limitation and coke formation often results in fast deactivation of the SSZ-39 zeolite *** solution for this challenge is to introduce mesoporosity in the SSZ-39 ***,we report the synthesis of mesoporous SSZ-39 zeolite using an organosilane surfactant,,-dimethyl--(3-(trimethoxysilyl)propyl)octan-1-aminium chloride,as a mesopore template and,-dimethyl--2,6-dimethylpiperidinium as a micropore *** obtained zeolites were characterized by X-ray diffraction,N sorption,scanning electron microscopy,temperature programmed desorption of ammonia,and magic angle spinning nuclear magnetic resonance of *** results show that the mesoporous SSZ-39 zeolite has high crystallinity,meso/microporosity,high surface area,cuboid morphology,and abundant acidic *** importantly,this mesoporous SSZ-39 zeolite exhibits enhanced catalyst lifetime in the MTO reaction due to the presence of mesoporosity for fast mass transfer,compared with a conventional SSZ-39 zeolite without mesoporosity.

关键词： SSZ-39 zeolite mesopores organosilane surfactant MTO reaction soft template mass transfer

The Mechanism of Phase Transition of Molecular Sieve VPI-5 into AlPO_4-8

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Chemical Research in Chinese Universities 1991年第3期7卷 174-175页

作者： Xu Yihua, xiao fengshou, Yao Shangqing, Liu Xinsheng and Pang Wengqin (Institute of Synthetic and Catalytic Chemistry, Jilin University, Changchun)

The aluminophosphate molecular sieve VPI-5 has received much attention as a new structure containing one-dimensional circular pores circumscribed by 18 tetrahedral atoms. The AlPO;-8 is another new type of structure which was found to contain 1 4-ring open pores. Recently, we have successfully synthesized the molecular sieves of VPI-5 and AlPO;-8, and found that the mixture of VPI-5 and AlPO;-8 was easily formed under similar conditions, and VPI-5 can be converted to AlPO;-8 by dehydration via heating. It is suggested that there exists relationship between the structures of VPI-5 and A1PO;-8. Therefore, the study on the transition and relationship between VPI-5 and A1PO;-8 is very important for designing and preparing new molecular sieves with new structures.

关键词： VPI-5 AlPO4-8 Topolygical framework Structure

Catalytic Performance and IR Characterization of Co-Mo/Al_2O_3 and Ru-Co-Mo/Al_2O_3 Catalysts in Hydrodesulfurization

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Chemical Research in Chinese Universities 1991年第3期7卷 172-173页

作者： xiao fengshou (Department of Chemistry,, Jilin University, Changchun)Xin Qin and Guo Xiexian (National Laboratory for Catalysis, Dalian Institute of Chemical Physics, Dalian)

Recently, owing to high costs and increasing demands for better catalysts, it is worthwhile to improve its activity and selectivity, and reduce its costs. Adding secondary promoters such as phosphorus, boron, magnesium, titanium, zinc and ruthenium to Co-Mo/Al;O;catalyst has been proved to be one of the ways to attain this result. The addition of those metals or metal oxides changes the surface states of molybdenumstructure.

关键词： Hydrodesulf urization IR spectra Ru-Co-Mo/Al2O3 Chemical adsorption

水滑石负载Au纳米粒子的制备及其催化醇氧化反应

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催化学报 2010年第8期31卷 943-947页

作者：王亮孟祥举肖丰收吉林大学无机合成与制备化学国家重点实验室吉林长春130012 浙江大学催化研究所浙江杭州310028

采用离子交换法和NaBH4还原法制备了Mg-Al-水滑石(LDH)负载的Au纳米粒子(Au/LDH)催化剂.X射线衍射和透射电镜结果表明,Au粒子较均匀地分散在水滑石表面,载体仍保持层状结构.在温和的反应条件下,Au/LDH对一系列醇的氧化反应表现出优异的... 详细信息

采用离子交换法和NaBH4还原法制备了Mg-Al-水滑石(LDH)负载的Au纳米粒子(Au/LDH)催化剂.X射线衍射和透射电镜结果表明,Au粒子较均匀地分散在水滑石表面,载体仍保持层状结构.在温和的反应条件下,Au/LDH对一系列醇的氧化反应表现出优异的催化性能,如在室温常压下进行分子O2氧化1-苯基乙醇的反应,底物转化率和苯乙酮选择性都接近100%,而且催化剂经过多次循环使用后,其活性未见下降.可见,Au/LDH催化剂在醇氧化反应中具有良好的应用前景.

关键词：金纳米粒子水滑石醇氧化分子氧

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无有机模板剂条件下合成沸石催化材料

催化学报 2009年第9期30卷 965-971页

作者：孟祥举谢彬肖丰收吉林大学无机合成与制备化学国家重点实验室吉林长春130012

工业上广泛应用的某些沸石催化材料,如ZSM-5和β沸石,通常是在有机模板剂存在条件下合成的,但合成过程常常会造成环境污染以及CO2和氮氧化物的排放.如果能在无有机模板剂条件下合成这些材料,则不仅在基础研究上具有重要意义,而且在工业... 详细信息

工业上广泛应用的某些沸石催化材料,如ZSM-5和β沸石,通常是在有机模板剂存在条件下合成的,但合成过程常常会造成环境污染以及CO2和氮氧化物的排放.如果能在无有机模板剂条件下合成这些材料,则不仅在基础研究上具有重要意义,而且在工业应用方面也具有经济和环保价值.本文对最近有关无有机模板剂合成沸石材料的一些突破性进展进行了综述,并重点讨论了调节起始凝胶配比、使用导向剂溶液以及使用晶种导向合成等路线.

关键词：沸石合成新路线有机模板剂凝胶配比导向剂溶液晶种

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分子筛催化反应中的凝聚态化学

化学进展 2023年第6期35卷 886-903页

作者：肖丰收吴勤明王成涛浙江大学化学工程与生物工程学院杭州310028

本文致力于讨论气固相的分子筛催化反应中的凝聚态化学,主要涉及:(i)气相中的反应物在分子筛孔道中的吸附;(ii)反应物在分子筛催化中心上的吸附与催化转化;(iii)反应产物从分子筛孔道中的脱附。在上述过程中,任何可以加快在分子筛上的... 详细信息

本文致力于讨论气固相的分子筛催化反应中的凝聚态化学,主要涉及:(i)气相中的反应物在分子筛孔道中的吸附;(ii)反应物在分子筛催化中心上的吸附与催化转化;(iii)反应产物从分子筛孔道中的脱附。在上述过程中,任何可以加快在分子筛上的反应物吸附、催化转化与反应产物脱附都可以提高分子筛催化材料的性能。为了实现这些目的,近年来人们提出了合成沸石催化材料的新策略,包括沸石晶体纳米化、引进介孔结构、制备沸石纳米片层和沸石晶体的浸润性调控。将具有催化功能的金属或金属氧化物物种引入到沸石晶体中,可以制备出结合沸石高稳定性与择形性以及高催化活性于一体的新型沸石催化材料,这对发展新的催化过程提供了新机遇。

关键词：凝聚态气固相催化反应沸石分子筛催化材料

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生物质基多元醇的多相催化选择性氢解

化学学报 2023年第5期81卷 533-547页

作者：刘露杰张建王亮肖丰收浙江大学化学工程与生物工程学院生物质化工教育部重点实验室北京化工大学软物质科学与工程高精尖创新中心

由生物质资源衍生得到的糖醇是一种可再生碳原料,并可以通过多相催化技术转化为高附加值的大宗化学品.因此,设计与制备具有高活性、高选择性和高稳定性的多相催化材料对于实现糖醇的定向转化具有重要意义.近年来,有关糖醇选择性氢解制... 详细信息

由生物质资源衍生得到的糖醇是一种可再生碳原料,并可以通过多相催化技术转化为高附加值的大宗化学品.因此,设计与制备具有高活性、高选择性和高稳定性的多相催化材料对于实现糖醇的定向转化具有重要意义.近年来,有关糖醇选择性氢解制备高附加值的一元醇、二元醇等已有许多报道,其中典型的Ir-ReOx和Pt-WOx催化剂在性能上有了进一步突破.此综述详细介绍了糖醇的选择性转化路径,并从金属-金属氧化物的相互作用、催化剂的构效关系和糖醇C—O键断裂的机理等方面进行归纳,并对糖醇定向转化的发展进行讨论与展望,这些对于新型多相催化材料的设计以及糖醇转化潜在的工业应用具有意义.

关键词：生物质基多元醇糖醇多相催化剂双功能催化剂加氢脱氧选择性氢解