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Trace Pd alloyed with Au to boost Au/uncalcined TS-1 catalyzed propane hydro-oxidation to acetone

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Nano Research 2024年第8期17卷 7182-7193页

作者： Jinwei Sun Zhihua Zhang Erchuan Yang Wei Du Fan Liu Kesheng Xu Yuxia Zhong Xuezhi Duan xinggui zhou State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Selective oxidation of propane to acetone(AC)with H_(2)and O_(2)provides a direct route to convert low-cost propane into valueadded ***,the catalytic activity of conventional Au/Ti-based catalysts is constrained by the high energy barrier for H_(2)***,uncalcined TS-1 supported Au-Pd bimetallic catalysts were prepared,and the relationship between the active-site structure and corresponding performance in the selective oxidation of propane with H_(2)and O_(2)in the gas phase was systematically *** contrast to the liquid-phase reaction,trace Pd alloyed with Au triggered an increase in both catalytic activity and selectivity,in which Au_(20)-Pd_(1)/TS-1-B catalyst exhibited excellent activity(170 gAC·h^(−1)·kgcat^(−1))and AC selectivity(90.6%),much higher than those of the Au/TS-1-B catalyst(AC formation rate of 100 gAC·h^(−1)·kgcat^(−1)and AC selectivity of 86.3%).It was found that Pd was gradually isolated into monomers with the increase of Au/Pd molar ratio,and the synergy between Pd single atoms and Au improved the catalytic performance via enhancing hydrogen dissociation and modulating the electronic structure of ***,the reaction conditions were optimized based on the kinetics studies and the Au_(20)-Pd_(1)/TS-1-B catalyst exhibited enhanced H_(2)selectivity(45%)and long-term stability(over 130 h).The insights gained here can offer valuable guidance for the design of Au-Pd catalysts applicable to other gas-phase oxidation reactions.

关键词： propane selective oxidation acetone hydrogen dissociation Au-Pd alloy synergy

Computational fluid dynamics simulation and experimental study on mixing performance of a three-dimensional circular cyclone-type microreactor

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Chinese Chemical Letters 2024年第4期35卷 382-388页

作者： Shiyu Hou Maolin Sun Liming Cao Chaoming Liang Jiaxin Yang xinggui zhou Jinxing Ye Ruihua Cheng School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China School of Pharmacy East China University of Science and TechnologyShanghai 200237China

Microchannels enable the fast and efficient mixing of multiphase *** this study, a millimeter-scale three-dimensional(3D) circular cyclone-type microreactor was designed for the *** flow characteristics and mixing intensity were simulated by computational fluid dynamics simulations at a flow rate range of 12–96 m L/min using a water/ethyl acetate *** the 3D variable-diameter structure,the microreactor induced paired opposite vortices and abruptly changed the local pressure to achieve a stable turbulent effect within the theoretical range of laminar *** injection simulations indicated that sufficient mixing units successfully promote fluid ***-coupling experiments showed a segregation index of X_S= 0.00,039 within a residence time of 9 *** experiments on the nbutanol/succinic acid/water system showed that the 3D circular cyclone-type microreactor achieved 100%extraction efficiency(E) in 4.25 s, and the overall volume mass transfer coefficient(K_La) reached 0.05–1.5s^(-1) in 12–96 m L/*** isolated yield of the phase transfer alkylation and oxidation reactions in the 3D circular cyclone-type microreactor achieved 99% within 36 s, which was superior to the coil microreactor and batch reactor.

关键词： Microfluidics Passive microreactor CFD simulation Extraction Liquid-liquid biphase reaction

Efficient continuous synthesis of 2-hydroxycarbazole and 4-hydroxycarbazole in a millimeter scale photoreactor

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Chinese Chemical Letters 2024年第4期35卷 399-403页

作者： Zhixiang Li Zhirong Yang Chang Yao Bin Wu Gang Qian Xuezhi Duan xinggui zhou Jing Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China

2-Hydroxycarbazole and 4-hydroxycarbazole are important chemicals with extensive applications in optoelectronic materials and pharmaceutical *** of the art yield of 2-hydroxycarbazole is~30%and the reaction time is typically in hours or ***,we developed a green route for the continuous and high-throughput synthesis of 2-hydroxycarbazole and 4-hydroxycarbazole via photochemical intramolecular cyclization of 3–hydroxy-2–chloro-diphenylamine using a self-designed millimeter scale photoreactor,which was designed based on sizing-up and numbering-up strategies for a decent liquid holdup(6.8 m L)and fabricated via femtosecond laser engraving *** photochemical synthesis was carried out continuously under the illumination of 365 nm UV-LED with dimethyl sulfoxide as solvent and potassium t-butoxide as *** was found that under optimized conditions a 2-hydroxycarbazole yield of 31.6%and a 4-hydroxycarbazole yield of 11.1%were obtained with a residence time of 1 *** to semibatch operations,the reaction time was shortened by 1–2 orders of *** a result,a throughput of 11.3 g/day 2-hydroxycarbazole and 4.0 g/day 4-hydroxycarbazole can be achieved from the *** was proposed that the short reaction time and high product yield are resulted from higher photon transfer rates and more uniform photon distribution provided by the millimeter scale photoreactor,which enhances the reaction rates and mitigates overreaction.

关键词： Millimeter scale reactor 2-Hydroxycarbazole Photochemistry UV-LED Process intensification

Poisoning effect of polyvinyl chloride on the catalytic pyrolysis of mixed plastics over zeolites

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Science China Chemistry 2024年第7期67卷 2265-2273页

作者： Jiangchun Yuan Wenjie Wang Weixiao Sun Zhirong Yang Yueqiang Cao Wenyao Chen Xiaohu Ge Gang Qian Xiang Feng Xuezhi Duan xinggui zhou Kevin M.Van Geem Jing Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Laboratory for Chemical Technology(LCT) Department of MaterialsTextiles and Chemical EngineeringFaculty of Engineering&ArchitectureGhent UniversityZwijnaarde B-9052Belgium State Key Lab of Heavy Oil Processing China University of PetroleumQingdao 266580China

Nowadays,the chemical recycling is applied for only 1%of total waste plastics,largely due to contaminants in plastic waste and difficulty in product *** the major contaminant,polyvinyl chloride(PVC)often forms corrosive hydrogen chloride(HCl)during the chemical recycling,which may cause severe catalyst deactivation and equipment ***,the investigation on catalytic pyrolysis(the major route for plastics chemical recycling)of the PVC containing mixed plastics has been rarely ***,catalytic co-pyrolysis of PVC and polyethylene(PE)was studied over an aromatization catalyst,Pt/ZSM-5,since the basic building block aromatics are desired products from plastics chemical *** poisoning effect of PVC vapor on the catalyst stability was explored by collective efforts of thorough product analysis and catalyst *** was found that the HCl evolving from PVC has an autocatalytic effect that promotes the scission of dehydrochlorinated PVC,resulting in the high yield of benzene and acetylene from *** the other hand,the presence of PVC suppressed the aromatics formation from PE,largely due to the poisoning effect of PVC-derived HCl on the Pt/*** deactivation is irreversible as evidenced by the decreased zeolite crystallinity and the loss of strong acid sites that are key to the aromatization,possibly due to the removal of framework Al upon the interaction with *** modification with octadecylphosphonic acid only slightly alleviated the PVC poisoning *** insights on the PVC poisoning of zeolite catalysts provided in this work may guide the process design of chemical recycling of PVC containing waste plastics.

关键词： polyvinyl chloride polyethylene zeolite aromatics deactivation

Micro/nano flow chemistry by Beyond Limits Manufacturing

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Chinese Chemical Letters 2024年第5期35卷 3-12页

作者： Peiwen Liu Fang Zhao Jing Zhang Yunpeng Bai Jinxing Ye Bo Bao xinggui zhou Li Zhang Changlu zhou Xinhai Yu Peng Zuo Jianye Xia Lian Cen Yangyang Yang Guoyue Shi Lin Xu Weiping Zhu Yufang Xu Xuhong Qian State Key Laboratory of Bioreactor Engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Bioreactor Engineering Shanghai Collaborative Innovation Center for BiomanufacturingEast China University of Science and TechnologyShanghai 200237China School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China School of Mechanical and Power Engineering East China University of Science and TechnologyShanghai 200237China Shanghai Key Laboratory of Green Chemistry and Chemical Processes Department of ChemistrySchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200241China

In September 2018,we proposed the cutting-edge concept of“Beyond Limits Manufacturing”(BLM).BLM technology is based on the three-dimensional inner engraving or precise outer engraving of ultra-fast laser,to invent micro/nano scale flow chips or devices,which makes it possible for the microform,integration,economy,safety,high efficiency,green and intelligence of research,development and manufacturing process,so as to realize transformational manufacturing in the era of Industry *** this paper,we reviewed the representative results we made in the field of micro/nano flow chemistry during the implementation of the BLM major project(December 2019 to August 2023),and discussed its application prospects in micro/nano flow chemistry.

关键词： Beyond Limits Manufacturing Flow chemistry Pharmaceutical manufacturing Microreactor

基于[bmim][BF_(4)]相转移催化的氟代碳酸乙烯酯高效合成

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化工学报 2024年第4期75卷 1543-1551页

作者：蒋方涛钱刚周兴贵段学志张晶华东理工大学化工学院化学工程联合国家重点实验室上海200237

氟代碳酸乙烯酯(FEC)是锂电池电解液添加剂的重要组分之一,其工业制备方法主要为卤素交换法,即氯代碳酸乙烯酯(CEC)与氟化钾(KF)通过取代反应制备FEC。该工艺中,取代反应速率受限于KF相际传质速率,且CEC易发生消去反应生成碳酸亚乙烯酯... 详细信息

氟代碳酸乙烯酯(FEC)是锂电池电解液添加剂的重要组分之一,其工业制备方法主要为卤素交换法,即氯代碳酸乙烯酯(CEC)与氟化钾(KF)通过取代反应制备FEC。该工艺中,取代反应速率受限于KF相际传质速率,且CEC易发生消去反应生成碳酸亚乙烯酯副产物。针对上述问题,研究了相转移催化剂(PTC)结构对KF相际传质速率和CEC制FEC主副反应能垒的影响规律和调控机制。优化条件下,PTC为[bmim][BF_(4)](1-丁基-3-甲基咪唑四氟硼酸盐),溶剂为乙腈,反应温度为乙腈回流温度(81.6℃),n(KF)∶n(CEC)=2.5∶1,此时FEC收率高达91.94%(摩尔分数)。密度泛函理论计算表明,在乙腈中[bmim][BF_(4)]能与KF形成配合物,增加K+和F-的核间距并降低KF的溶解自由能,从而强化相际传质并降低取代反应能垒,实现CEC经KF取代高效制备FEC。

关键词：离子液体相转移催化配合物传质氟代碳酸乙烯酯密度泛函理论

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氧化铝结构与表面性质调控及其催化甲醇脱水制二甲醚性能研究

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化工学报 2024年第7期75卷 2522-2532页

作者：罗莉陈文尧张晶钱刚周兴贵段学志华东理工大学化工学院化学工程联合国家重点实验室上海200237

二甲醚(DME)作为一种关键的化工原料,被广泛用于合成众多重要的化学品及能源产品。在工业生产中用于从甲醇制备DME的催化剂γ-Al_(2)O_(3)因其高效的催化性能而得到普遍应用。然而,γ-Al_(2)O_(3)的合成方法和制备条件对其催化性能有着... 详细信息

二甲醚(DME)作为一种关键的化工原料,被广泛用于合成众多重要的化学品及能源产品。在工业生产中用于从甲醇制备DME的催化剂γ-Al_(2)O_(3)因其高效的催化性能而得到普遍应用。然而,γ-Al_(2)O_(3)的合成方法和制备条件对其催化性能有着显著的影响。目前,对于工业上常用的γ-Al_(2)O_(3)合成条件如何影响其催化性能的系统研究仍然不足。特别是,作为影响催化性能的关键因素之一,酸性位点的性质尚未形成共识。通过调控双铝法成胶过程中母液的pH,成功合成了一系列具有不同孔道结构和酸性质的γ-Al_(2)O_(3)。实验结果表明,随着母液pH的增大,γ-Al_(2)O_(3)的比表面积、孔容和孔径均呈现减小趋势。同时,γ-Al_(2)O_(3)的弱酸量逐渐减小,而中强酸量呈现先增后减的趋势。进一步结合催化性能评估结果,发现中强酸数量与甲醇脱水性能密切相关。具有最高中强酸数量的γ-Al_(2)O_(3)表现出最高的DME产率,预示中强酸位点是γ-Al_(2)O_(3)催化甲醇脱水制备DME的主要活性中心。针对具有最优性能的γ-Al_(2)O_(3)开展动力学实验分析,得到甲醇脱水的反应级数为0.78,反应活化能为83.27 kJ/mol。研究可为甲醇脱水制备DME催化剂的设计提供指导,为进一步优化工业生产条件和提高催化效率夯实基础。

关键词：氧化铝甲醇脱水二甲醚酸性调控催化剂动力学

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新型欧姆加热式反应器强化甲烷蒸汽重整的过程分析和优化

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低碳化学与化工 2024年第1期49卷 76-84页

作者：高贤清宋楠叶光华周兴贵华东理工大学化工学院化学工程联合国家重点实验室上海200237

传统甲烷蒸汽重整(SMR)反应器(cSMR反应器)中容易出现较大的径向温度梯度,增加了催化剂积炭失活的风险。提出了一种新型的含内外管欧姆加热蒸汽重整固定床反应器(eSMR反应器),以欧姆加热替代了传统工业反应器的燃烧供热方式。通过二维... 详细信息

传统甲烷蒸汽重整(SMR)反应器(cSMR反应器)中容易出现较大的径向温度梯度,增加了催化剂积炭失活的风险。提出了一种新型的含内外管欧姆加热蒸汽重整固定床反应器(eSMR反应器),以欧姆加热替代了传统工业反应器的燃烧供热方式。通过二维拟均相固定床反应器模拟,比较了eSMR与cSMR反应器的性能差异,分析了eSMR反应器结构及操作条件对其性能的影响。结果表明,相比于cSMR,eSMR反应器出口的平均甲烷转化率和平均温度分别高出26.6%和121 K,且径向温度分布更加均匀;eSMR反应器的内外管直径之比为0.589时,其径向温度梯度最小;增加入口温度、加热电压和水碳比均会提高eSMR反应器出口的平均甲烷转化率和平均温度,增加入口压力的影响相反。本研究可为欧姆加热蒸汽重整反应器的开发提供一定的借鉴。

关键词：欧姆加热甲烷蒸汽重整固定床反应器数学模型优化设计

Probing deactivation by coking in catalyst pellets for dry reforming of methane using a pore network model

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Chinese Journal of Chemical Engineering 2023年第3期55卷 293-303页

作者： Yu Wang Qunfeng Zhang Xinlei Liu Junqi Weng Guanghua Ye xinggui zhou State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, which prevents this technology from commercialization. In this work, a pore network model is developed to probe the catalyst deactivation by coking in a Ni/Al_(2)O_(3) catalyst pellet for DRM. The reaction conditions can significantly change the coking rate and then affect the catalyst deactivation. The catalyst lifetime is higher under lower temperature, pressure, and CH_(4)/CO_(2) molar ratio, but the maximum coke content in a catalyst pellet is independent of these reaction conditions. The catalyst pellet with larger pore diameter, narrower pore size distribution and higher pore connectivity is more robust against catalyst deactivation by coking, as the pores in this pellet are more difficult to be plugged or *** maximum coke content is also higher for narrower pore size distribution and higher pore connectivity, as the number of inaccessible pores is lower. Besides, the catalyst pellet radius only slightly affects the coke content, although the diffusion limitation increases with the pellet radius. These results should serve to guide the rational design of robust DRM catalyst pellets against deactivation by coking.

关键词： Deactivation by coking Dry reforming of methane Pore network model Diffusion limitation Catalyst pellet