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构筑开放锡位点实现酸性增强的二甲醚羰基化丝光沸石催化剂设计

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Engineering 2024年第4期35卷 104-114页

作者： Ying Li man Yu Guodong Qi Yunduo Liu Jing Lv Shouying Huang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China National Center for magnetic Resonance in Wuhan&State Key Laboratory of magnetic Resonance and Atomic and Molecular Physics&Key Laboratory of magnetic Resonance in Biological Systems Wuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071China Inner Mongolia Key Laboratory of Industrial Catalysis College of Chemical EngineeringInner Mongolia University of TechnologyHohhot 010051China

Due to their tunable acidity,shape selectivity,and excellent stability,zeolites are of great importance as solid acid materials in industrial *** the properties of the acid sites in zeolites allows for the rational design and fabrication of catalysts for target *** ether(DME)carbonylation,a critical chain-growth reaction for C1 resource utilization,is selectively catalyzed by the Brønsted acid sites within the eight-membered rings(8-MRs)of mordenite(MOR).It is anticipated that strengthening the Brønsted acidity—particularly in 8-MRs—will improve the catalytic performance of *** this work,density functional theory(DFT)calculations are first employed and the results used to design a modified MOR with stannum(Sn)and to predict the corresponding changes in *** by the theoretical studies,a series of Sn-modified MOR are synthesized via a defect-engineering and subsequent heteroatom-substitution *** partial desilication,isolated tetrahedral Sn species in an open configuration are successfully synthesized for the first time,within which tetrahedrally coordinated Al sites are *** acidic characterization is used to confirm that the acidity of the Brønsted acid sites is enhanced by the introduction of the Sn species;as a result,the sample exhibits excellent activity in DME carbonylation *** and DFT studies reveal that this strengthened acidity facilitates the adsorption of DME and reduces the activation barriers of DME dissociation and acetyl formation,accounting for the improved *** work demonstrates mechanistic insights into the promoting effects of strong acidity on DME carbonylation and offers a promising strategy to precisely control the acidic strength of zeolites.

关键词： Zeolite Sn modification Carbonylation Brønsted acid catalysis Acidic strength

外生冲击、投资构成与经济增长——基于供给侧与需求侧的双重视角

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武汉大学学报（哲学社会科学版） 2024年第4期77卷 114-127页

作者：汪勇马新彬中国社会科学院金融研究所北京100710 中国人民银行北京100045

进入新发展阶段,我国经济正处于新旧动能转换关键期,外部环境不确定性、不稳定性增加,稳增长、促发展、调结构压力较大,强化宏观政策对高质量发展的统筹支持十分关键。研发补贴等供给侧政策,短期内对稳增长的作用较弱,但能够推动企业提... 详细信息

进入新发展阶段,我国经济正处于新旧动能转换关键期,外部环境不确定性、不稳定性增加,稳增长、促发展、调结构压力较大,强化宏观政策对高质量发展的统筹支持十分关键。研发补贴等供给侧政策,短期内对稳增长的作用较弱,但能够推动企业提高研发投资占比,提升经济增长潜力,这一效应随着研发外溢效应的上升而不断增强。与此不同,居民消费补贴等需求侧政策,长期内持续推动经济增长的作用相对有限,但短期内促进固定资产投资、稳定经济增长的作用突出,该效应在资本产出弹性下降时会进一步凸显。推动经济高质量发展,要充分发挥供需政策促进长短期经济增长的合力。

关键词：投资构成经济增长内生技术进步宏观政策

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非均相单宁酸-锆介孔材料制备及其CO_(2)环加成反应催化性能

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化工进展 2024年第5期43卷 2803-2810页

作者：冯帮满岳成光王美岩王悦马新宾天津大学化工学院天津300350 天津大学浙江研究院浙江宁波315201

CO_(2)和环氧化物的环加成反应是一种有效且可持续的CO_(2)化工转化策略,其产品环碳酸酯在锂离子电池、高分子材料等领域具有广泛应用。其中环氧化物的开环被认为是该反应的关键步骤,因此构筑具有高效环氧化物吸附活化位点的催化剂至关... 详细信息

CO_(2)和环氧化物的环加成反应是一种有效且可持续的CO_(2)化工转化策略,其产品环碳酸酯在锂离子电池、高分子材料等领域具有广泛应用。其中环氧化物的开环被认为是该反应的关键步骤,因此构筑具有高效环氧化物吸附活化位点的催化剂至关重要。本文通过单宁酸与锆离子的配位作用,“一锅法”制备同时含有锆金属中心作为Lewis酸位点和酚羟基作为氢键作用位点的非均相单宁酸-锆介孔材料TA-Zr-2。XPS和环氧丙烷TPD-MS结果表明,与同为锆基多孔材料的UiO-66相比,TA-Zr-2的锆金属中心具有更强的Lewis酸性,对环氧丙烷具有更强的吸附活化作用。在TA-Zr-2的基础上通过冷冻干燥优化处理得到了具有更大比表面积和合适孔体积的TA-Zr-2-FD材料,25℃下催化性能提升1倍,24h的碳酸丁烯酯收率达97.6%。本文使用简单绿色的制备方法,构建了具有较大比表面积的单宁酸-锆介孔材料,锆Lewis酸位点和酚羟基氢键位点的耦合使其具有良好的环氧化物吸附活化作用,利于环氧化物的开环,使得该催化剂在25℃下表现出良好的CO_(2)环加成反应催化性能。

关键词： CO_(2)转化环加成反应环状碳酸酯介孔材料

多位点离子液体聚合物催化CO2环加成反应研究

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化学工业与工程 2024年第2期41卷 2-11页

作者：王昊岳成光王美岩马新宾天津大学化工学院

CO2与环氧化物环加成反应制备环状碳酸酯是一条绿色经济的CO2利用途径。针对现有CO2与环氧化物环加成反应中非均相离子液体催化剂活性低和活性组分易流失等问题，设计制备了系列多位点离子液体超交联聚合物HCPs-[DmPhe]Br,研究了多位点... 详细信息

CO2与环氧化物环加成反应制备环状碳酸酯是一条绿色经济的CO2利用途径。针对现有CO2与环氧化物环加成反应中非均相离子液体催化剂活性低和活性组分易流失等问题，设计制备了系列多位点离子液体超交联聚合物HCPs-[DmPhe]Br,研究了多位点协同作用、超交联聚合物组成和结构等因素对其催化CO2与环氧化物环加成反应性能的影响。其中，同时含有双季铵-卤素离子对、羟基和叔胺结构的HCP-[DmPhe]Br-DCX离子液体超交联聚合物催化剂，在1.3 MPa, 130℃,8 h的条件下，可实现94%的碳酸丁烯酯收率，且催化剂循环稳定性好，重复使用5次，催化活性没有明显降低。另外，超交联聚合物的多孔结构以及大比表面积促进了离子液体的较好分散，使其与离子液体单体具有相当的活性。该工作对CO2与环氧化物环加成反应高效非均相离子液体催化剂的开发与优化具有一定的借鉴意义。

关键词： CO2利用环状碳酸酯离子液体协同作用超交联聚合

High-temperature CO_(2) sorbents with citrate and stearate intercalated Ca-Al hydrotalcite-like as precursor

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Chinese Journal of Chemical Engineering 2022年第10期50卷 177-184页

作者： Tao Jiang Fei Xiao Yujun Zhao Shengping Wang xinbin ma Key Laboratory for Green Chemical Technology School of Chemical Engineering and TechnologyCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China

CO_(2),one of the main components of greenhouse gases,increased rapidly because of the growing use of fossil *** CaO sorbents possess the capability to be used in capture of CO_(2) at high *** the work,Ca-Al complex oxides derived from citrate and stearate intercalated layered double hydroxides were fabricated and their CO_(2) adsorption capacity was compared with that from CO_(3)^(2-)intercalated layered double *** results presented that the sorbents(Ca/Al=5)with Ca-Al-citrate layered double hydroxides as precursors performed best and displayed remarkable CO_(2) capture capacity of 52.0%(mass)at the carbonization temperature of 600℃without distinct recession during cycling adsorption/desorption *** excellent CO_(2) adsorption capacity of the sorbent was ascribed to its smaller crystallite size of calcinated particles,optimized pore size distribution as well as homogeneous distributed Ca and Al in the sorbent.

关键词： Layered doublehydroxides CO_(2)capture CaO-based Organic ions

SSZ-13分子筛在二甲醚羰基化反应中的机理研究和空间限域效应

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Chinese Journal of Catalysis 2024年第6期61卷 301-311页

作者：张晓敏蔡凯李媖戚暨王悦刘云铎王美岩黄守莹马新宾天津大学化工学院绿色合成与转化教育部重点实验室物质绿色创造与制造海河实验室天津300350 天津大学浙江研究院浙江宁波315201 中石化石油化工科学研究院有限公司北京100083 内蒙古工业大学化工学院内蒙古呼和浩特010051 天津大学分子+研究院天津300350

乙醇作为一种绿色清洁的燃料替代品和油品添加剂,在全球有广泛的市场需求.利用合成气经乙酸甲酯(ma)合成乙醇的工艺路线,因其原子经济性、产品选择性高、反应条件温和等优势而备受关注.其中,二甲醚(DME)羰基化是该路线的关键步骤之一.... 详细信息

乙醇作为一种绿色清洁的燃料替代品和油品添加剂,在全球有广泛的市场需求.利用合成气经乙酸甲酯(ma)合成乙醇的工艺路线,因其原子经济性、产品选择性高、反应条件温和等优势而备受关注.其中,二甲醚(DME)羰基化是该路线的关键步骤之一.研究证实,具有8元环(8-MR)孔道结构的硅铝酸盐微孔分子筛可以在较低的反应温度下高选择性催化二甲醚羰基化反应.目前,研究者已经对丝光沸石(MOR)、镁碱沸石(FER)等分子筛进行了全面深入的分析,但对SSZ-13等菱沸石(CHA型)的研究有限,缺乏SSZ-13上主、副反应催化机理的阐释,并且忽略了沸石独特的笼状结构在反应中的空间限域效应.本文结合实验和理论计算确定了SSZ-13分子筛催化DME羰基化的活性位点,并探究了孔道的限域效应.通过负载具有不同尺寸的Na^(+)和Cs^(+)实现了对不同通道中Brönsted酸位点(BAS)的选择性屏蔽.酸性质表征和密度泛函理论(DFT)计算结果表明,在较低的负载量下,Na^(+)优先取代SSZ-13的6元环(6-MR)中的BAS,而Cs^(+)由于其较大的离子半径只能与8-MR中的BAS发生交换,从而实现了对SSZ-13不同孔道中酸分布的调控.负载不同金属量以及金属种类的样品活性研究表明,当6-MR中BAS减少时,DME转化率基本不变;而当8-MR中BAS被离子交换时,DME转化率明显下降.随后,将未经金属改性的、具有不同硅铝比的母体SSZ-13样品的ma生成速率与其8-MR中BAS的数量相关联,发现两者呈较好的线性关系,说明SSZ-13的8-MR中BAS为DME羰基化的活性中心.同时,DFT计算了DME在不同孔道BAS上的解离能,结果表明DME更容易在8-MR的BAS上解离从而进行后续反应.随后,探究了SSZ-13笼的空间限域效应对主副反应的影响机制.通过比较金属负载量相近的Na/H-SSZ-13和Cs/H-SSZ-13上CO插入甲氧基形成烯酮的反应势垒,证实了较大尺寸金属离子的引入增加了主反应速控步的能垒.为了揭示空间限域对副反应的影响,比较了反应后催化剂的热重、气质联用等表征结果,并利用密度泛函理论计算了副反应的关键物种(七甲基苯正离子)在Na/H-SSZ-13和Cs/H-SSZ-13上的吸附能,证实了SSZ-13的笼状结构体积是影响ma选择性的关键因素.金属负载后SSZ-13笼空间减少,可以有效地抑制副反应关键物种的形成,从而提高主反应选择性.综上,本文不仅对SSZ-13分子筛催化二甲醚羰基化反应机理进行了全面解析,并通过实验设计,改变了SSZ-13分子筛的孔道结构和笼结构空间,突出了分子筛限域效应在二甲醚羰基化反应中的重要作用.本文研究结果为设计具有较高选择性的沸石催化剂提供一定的参考.

关键词：二甲醚羰基化 SSZ-13分子筛酸位点限域效应

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

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Frontiers of Chemical Science and Engineering 2022年第3期16卷 397-407页

作者： Deng Pan Jiahua Zhou Bo Peng Shengping Wang Yujun Zhao xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin300072China SINOPEC Research Institute of Petroleum Processing(RIPP) Beijing100083China

The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of ***,a series of Ni-doped PtSn catalysts were prepared,characterized and studied in the hydrogenation of acetic *** Ni dopant has a strong interaction with Pt,which promotes the hydrogen adsorption,providing an activated hydrogen-rich environment for the ***,the presence of Ni also improves the Pt dispersion,giving more accessible active sites for hydrogen *** cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to *** a result,the catalyst with 0.1%Ni exhibits the best reaction activity,and its space time yield is twice as that of the PtSn/SiO2 *** provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.

关键词： acetic acid ethanol hydrogenation Pt Ni cooperation effect

Coupling effect of bifunctional ZnCe@SBA-15 catalyst in 1,3-butadiene production from bioethanol

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Chinese Journal of Chemical Engineering 2022年第5期35卷 162-170页

作者： Zheng Wang Sijia Li Shengping Wang Jiaxu Liu Yujun Zhao xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin 300072China State Key Laboratory of Fine Chemicals Department of Catalytic Chemistry and EngineeringDalian University of TechnologyDalian 116024China

A series of bifunctional Zn Ce@SBA-15 catalysts with different Zn/Ce ratios were prepared by a solid-state grinding strategy and used in the conversion of ethanol to 1,3-butadiene(ETB).For the supported metal oxides,Zn O serves as the active sites for the dehydrogenation of ethanol,and CeO_(2) promotes the aldolcondensation *** on the results of Py-FTIR and NH_(3)-TPD,it suggests that the yield of 1,3-butadiene is positively correlated with the number of weak Lewis acid sites on the catalyst surface,given their benefit for aldol-condensation *** catalyst with an optimal Zn/Ce ratio of about 1:5 has the highest concentration of weak Lewis *** with the Zn O sites,it contributes to a 98.4%conversion of ethanol and a 45.2%selective of 1,3-butadiene under relatively mild reaction conditions(375°C,101.325 k Pa,and 0.54 h^(-1)).

关键词： Biomass Catalyst Coupling effect Lewis acid 1 3-butadiene Optimization

Progress in Processes and Catalysts for Dehydrogenation of Cyclohexanol to Cyclohexanone

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Transactions of Tianjin University 2023年第3期29卷 196-208页

作者： Jing Gong Shixin Hou Yue Wang xinbin ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

The dehydrogenation of cyclohexanol to cyclohexanone is a crucial industrial process in the production of caprolactam and adipic acid, both of which serve as important precursors in nylon textiles. This endothermic reaction is constrained by thermodynamic equilibrium and involves a complex reaction network, leading to a heightened focus on catalysts and process design. Copper-based catalysts have been extensively studied and exhibit exceptional low-temperature catalytic performance in cyclohexanol dehydrogenation, with some being commercially used in the industry. This paper specifically concentrates on research advancement concerning active species, reaction mechanisms, factors influencing product selectivity, and the deactivation behaviors of copper-based catalysts. Moreover, a brief introduction to the new processes that break thermodynamic equilibrium via reaction coupling and their corresponding catalysts is summarized here as well. These reviews may off er guidance and potential avenues for further investigations into catalysts and processes for cyclohexanol dehydrogenation.

关键词： Cyclohexanol Dehydrogenation Cyclohexanone Copper-based catalyst Reaction coupling processes