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Tuning the cross-linked structure of basic poly(ionic liquid)to develop an efficient catalyst for the conversion of vinyl carbonate to dimethyl carbonate

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Chinese Journal of Chemical Engineering 2024年第8期72卷 106-116页

作者： Zhaoyang Qi Shiquan Zhong Huiyun Su Changshen Ye Limei Ren Ting Qiu Jie Chen College of Chemical Engineering Fuzhou UniversityFuzhou 350108China Department of Chemical Engineering Shijiazhuang UniversityShijiazhuang 050035China qingyuan innovation laboratory Quanzhou 362801China Fuzhou University International Joint laboratory of Thermochemical Conversion of Biomass Fuzhou UniversityFuzhou 350108China

Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other *** current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and ***,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and *** address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and *** poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic *** was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing *** was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant *** results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.

关键词： Poly(ionic liquid) Cross-linking degree Dimethyl carbonate production Transesterification reaction Mechanism

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Controlling reversible complexation-mediated polymerization(RCMP)via deep eutectic solvents:fast kinetics,narrow molecular weight distribution and mechanistic insights

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Science China Chemistry 2024年第8期67卷 2728-2736页

作者： Xin Fu Zhen Lu Shen Li Zheng-Hong Luo Lin-Xi Hou Department of Materials-Oriented Chemical Engineering College of Chemical EngineeringFuzhou UniversityFuzhou 350116China Department of Chemical Engineering School of Chemistry and Chemical EngineeringState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200030China Chemical Engineering Zhicheng College of Fuzhou UniversityFuzhou 350116China qingyuan innovation laboratory Quanzhou 362801China

The exploitation of new green polymerization avenues for the effective synthesis of polymers by reversible-deactivation radical polymerization plays a critical role in pursuing the development of polymeric *** this work,serials of deep eutectic solvents(DES)with intermolecular-hydrogen-bonding interaction were constructed as catalysts and medium for actuating reversible complexation-mediated polymerization(RCMP)for the first time,yielding methacrylate polymers with high monomer conversion and narrow dispersion molecular weight in both water and oil *** mechanism and elementary reaction of RCMP were explored deeply,revealing that the complexation of initiator with DES to generate radicals was a ratecontrolling step and intermolecular-hydrogen-bond was primary factor to influence polymerization ***,the insights of density functional theory calculations revealed that negative electrostatic potential ensured nucleophilic *** investigation demonstrated the considerable potential of DES for RCMP,which is anticipated for other polymerization applications as a novel medium mode.

关键词： deep eutectic solvent reversible complexation-mediated polymerization intermolecular hydrogen bonding density functional theory elementary reaction steps

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Utilizing dual-responsive iridium(Ⅲ) complex for hepatocellular carcinoma: Integrating photoacoustic imaging with chemotherapy and photodynamic therapy

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Chinese Chemical Letters 2024年第9期35卷 296-302页

作者： Jinyu Guo Yandai Lin Shaohua He Yueqing Chen Fenglu Li Renjie Ruan Gaoxing Pan Hexin Nan Jibin Song Jin Zhang qingyuan innovation laboratory Quanzhou 362801China College of Chemical Engineering Fuzhou UniversityFuzhou 350108China MOE key laboratory for Analytical Science of Food Safety and Biology State Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350108China Department of Pediatric Surgery Shengli Clinical Medical College of Fujian Medical UniversityFuzhou 350001China

Stimuli-triggered release and alleviating resistance of iridium(Ⅲ)-based drugs at tumor sites remains challengeable for clinical hepatoma ***,a doxorubicin@iridium-transferrin(DOX@Ir-TF)nanovesicle was synthesized by carboxylated-transferrin(TF)and doxorubicin-loaded amphiphilic iridium-amino with quaternary ammonium(QA)groups and disulfide *** QA groups enhanced photophysical properties and broadened production capacity of photoinduced-reactive oxygen species(ROS),while the disulfide-bridged bonds regulated oxidative stress levels through reacting with glutathione(GSH);simultaneously,modification of TF improved recognition and endocytosis of the nanovesicle for tumor *** on in-vitro results,a controlled-release behavior of DOX upon a dualresponsiveness of GSH and near-infrared ray(NIR)irradiation was presented,along with high-efficiency generation of *** an intravenous injection,the nanovesicle was targeted at tumor sites,realizing TF-navigated photoacoustic imaging guidance and synergistic chemotherapy-photodynamic therapy under NIR/GSH ***,newly-synthesized DOX@Ir-TF nanovesicle provided a potential in subcutaneous hepatocellular carcinoma therapy due to integrations of targeting delivery,dual-stimuli responsive release,synergistic therapy strategy,and real-time monitoring.

关键词： Amphiphilic iridium complex Transferrin targeting NIR/GSH dual-responsiveness Photoacoustic imaging Synergistic tumor therapy

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Utilizing dual-responsive iridium(Ⅲ) complex for hepatocellular carcinoma: Integrating photoacoustic imaging with chemotherapy and photodynamic therapy

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Chinese Chemical Letters 2024年第09期 322-328页

作者： Jinyu Guo Yandai Lin Shaohua He Yueqing Chen Fenglu Li Renjie Ruan Gaoxing Pan Hexin Nan Jibin Song Jin Zhang qingyuan innovation laboratory College of Chemical Engineering Fuzhou University Department of Pediatric Surgery Shengli Clinical Medical College of Fujian Medical University MOE key laboratory for Analytical Science of Food Safety and Biology State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University

Stimuli-triggered release and alleviating resistance of iridium(III)-based drugs at tumor sites remains challengeable for clinical hepatoma therapy. Herein, a doxorubicin@iridium-transferrin(DOX@IrTF) nanovesicle was synthesized by carboxylated-transferrin(TF) and doxorubicin-loaded amphiphilic iridium-amino with quaternary ammonium(QA) groups and disulfide bonds. The QA groups enhanced photophysical properties and broadened production capacity of photoinduced-reactive oxygen species(ROS), while the disulfide-bridged bonds regulated oxidative stress levels through reacting with glutathione(GSH); simultaneously, modification of TF improved recognition and endocytosis of the nanovesicle for tumor cells. Based on in-vitro results, a controlled-release behavior of DOX upon a dualresponsiveness of GSH and near-infrared ray(NIR) irradiation was presented, along with high-efficiency generation of ROS. After an intravenous injection, the nanovesicle was targeted at tumor sites, realizing TF-navigated photoacoustic imaging guidance and synergistic chemotherapy-photodynamic therapy under NIR/GSH stimulations. Overall, newly-synthesized DOX@Ir-TF nanovesicle provided a potential in subcutaneous hepatocellular carcinoma therapy due to integrations of targeting delivery, dual-stimuli responsive release, synergistic therapy strategy, and real-time monitoring.

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Impacts of support properties on the vacuum residue slurry-phase hydrocracking performance of Mo catalysts

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Petroleum Science 2023年第4期20卷 2575-2584页

作者： Wei-Wei Feng Ye-Gui Qian Ting-Hai Wang Qing-Yan Cui Yuan-Yuan Yue Pei Yuan Xiao-Jun Bao College of Chemical Engineering Fuzhou UniversityFuzhouFujian350116China qingyuan innovation laboratory QuanzhouFujian362801China

To deeply understand the effects of support properties on the performance of Mo-based slurry-phase hydrocracking catalysts,four Mo-based catalysts supported on amorphous silica alumina(ASA),γ-Al_(2)O_(3),ultra-stable Y(USY)zeolite and SiO_(2) were prepared by the incipient wetness impregnation method,respectively,and their catalytic performances were compared in the vacuum residue(VR)hydrocracking *** is found that the Mo/ASA catalyst exhibits the highest VR conversion among the different catalysts,indicating that both the appropriate amount of acid sites,especially B acid sites and larger mesoporous volume of ASA can enhance the VR hydrocracking into light ***,Mo catalysts supported on the different supports show quite different product distributions in VR *** Mo/ASA catalyst provides higher yields of naphtha and middle distillates and lower yields of gas and coke compared with other catalysts,it is attributed to the highest MoS_(2) slab dispersion,the highest sulfuration degree of Mo species,and the most Mo atoms located at the edge sites for the Mo/ASA catalyst,as observed by HRTEM and XPS *** features of Mo/ASA are beneficial for the hydrogenation of intermediate products and polycyclic aromatic hydrocarbons to restrict the gas and coke formation.

关键词： Slurry-phase hydrocracking Vacuum residue Supports Catalytic performance

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Styrene epoxidation catalyzed by polyoxometalate/quaternary ammonium phase transfer catalysts: The effect of cation size and catalyst deactivation mechanism

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Chinese Journal of Chemical Engineering 2023年第3期55卷 192-201页

作者： Qiongna Xiao Yuyan Jiang Weiqiang Yuan Jingjing Chen Haohong Li Huidong Zheng College of Chemical Engineering Fuzhou UniversityFuzhou 350116China qingyuan innovation laboratory Quanzhou 362801China Engineering Research Center of Advanced Manufacturing Technology for Fine Chemicals Fujian Province UniversityFuzhou UniversityFuzhou 350116China College of Chemistry Fuzhou UniversityFuzhou 350116China

Catalytic epoxidation of alkenes is an important type of organic reaction in chemical industry,and the deep insight into catalyst deactivation will help to develop new epoxidation *** this work,series of quaternary ammoniums bearing different cationic sizes,***+(methyltrioctylammonium,[(C_(8)H_(17))_(3)CH_(3)N]+),HTMA+(hexadecyltrimethylammonium,[(C_(16)H_(33))(CH_(3))_(3)N]+) and DMDOA+(dimethyldioctadecylammonium,[(C_(18)H_(37))_(2)(CH_(3))_(2)N]+) were incorporated with polyoxometalate (POM) anions to prepare phase transfer catalysts (PTCs),which were used in the styrene *** them,(MTOA)_(3)PW_(4)O_(24)exhibits the best catalytic performance judged from the highest styrene conversion rate(52%) and styrene oxide selectivity (93%),during which the styrene epoxidation conditions were ***,the deactivation mechanism of this kind of PTCs was proposed firstly,*** the case of low H_(2)O_(2) content,the oxidant can only be used in the styrene epoxidation,in which the catalyst can transform into stable Keggin-type *** when the content of H_(2)O_(2) is higher,the excess H_(2)O_(2) can reactivate the Keggin-type POM into active (PW_(4)O_(24))_(3)-anions,which can trigger the ring-opening polymerization of styrene ***,the catalyst is deactivated by adhered poly(styrene oxide)irreversibly,which was determined by NMR *** this situation,the active moiety{PO_(4)[WO(O_(2))_(2)]_(4)}_(3)-in phase-transfer catalytic system can break into some unidentified species with low W/P ratio with the presence of *** work will be beneficial for the design of new PTCs in alkene epoxidation in fine chemical industry.

关键词： Phosphotungstic acid phase-transfer catalyst Styrene epoxidation Catalyst deactivation mechanism Cation size effect

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Kinetics measurement of ethylene-carbonate synthesis via a fast transesterification by microreactors

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Chinese Journal of Chemical Engineering 2023年第1期53卷 243-250页

作者： Tengjie Wang Wenkai Li Xuehui Ge Ting Qiu Xiaoda Wang Engineering Research Center of Reactive Distillation Fujian Province Higher Education InstitutesCollege of Chemical EngineeringFuzhou UniversityFuzhou 350108China Qingyuan Innovation LaboratoryQuanzhou 362801China

High-purity ethylene carbonate(EC)is widely used as battery electrolyte,polycarbonate monomer,organic intermediate,and so *** economical and sustainable route to synthesize high-purity ethylene carbonate(EC)via the transesterification of dimethyl carbonate(DMC)with ethylene glycol(EG)is provided in this ***,this reaction is so fast that the reaction kinetics,which is essential for the industrial design,is hard to get by the traditional measuring *** this work,an easy-to-assemble microreactor was used to precisely determine the reaction kinetics for the fast transesterification of DMC with EG using sodium methoxide as *** effects of flow rate,microreactor diameter,catalyst concentration,reaction temperature,and reactant molar ratio were *** activity-based pseudohomogeneous kinetic model,which considered the non-ideal properties of reaction system,was established to describe the transesterification of DMC with *** kinetics data were collected in the first 5 *** these data,the parameters of the kinetic model were correlated with the maximum average error of 11.19%.Using this kinetic model,the kinetic data at different catalyst concentrations and reactant molar ratios were predicted with the maximum average error of 13.68%,suggesting its satisfactory prediction performance.

关键词： Microreactor Kinetics Ethylene carbonate synthesis Transesterification Sodium methoxide

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Stimuli-responsive emulsions:Recent advances and potential applications

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Chinese Journal of Chemical Engineering 2022年第1期35卷 193-209页

作者： Xue-hui Ge Liangji Mo Anhe Yu Chenzi Tian Xiaoda Wang Chen Yang Ting Qiu Engineering Research Center of Reactive Distillation Fujian Province UniversityCollege of Chemical EngineeringFuzhou UniversityFuzhou 350108China qingyuan innovation laboratory Quanzhou 362801China

Responsive emulsions are the emulsions that can be reversibly switched on-demand between“stable”and“unstable”by environmental stimulus or trigger,which allows a simple and effective adjustment approach to achieve emulsification and *** recent years,stimuli-responsive emulsions acting as smart soft material are received considerable attention with the advantages of simple manipulation,good reversibility,low cost,easy treatment,and little effect on the *** this paper,the recent research progress of emulsions that can respond to external stimuli,including pH,light,magnetic field,CO_(2)/N_(2) and dual responsive are ***,the potential applications based on responsive emulsion are discussed,such as catalytic reactions,heavy oil recovery,polymer particles synthesis and optical sensor,aiming to summarize the latest achievements and put forward the possible development trends of responsive emulsions.

关键词： Stimuli-responsive Emulsions Switchable surfactants Interface

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Reversible Chain Transfer Catalyzed Polymerization with Alkyl Iodides Generated from Alkyl Bromides by in Situ Halogen Exchange

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Chinese Journal of Polymer Science 2021年第9期39卷 1161-1168页

作者： Dan-Ni Gao Yu-Lai Zhao Jing-Yu Cai Lin-Xi Hou Long-Qiang Xiao Department of Materials-Oriented Chemical Engineering School of Chemical EngineeringFuzhou UniversityFuzhou 350116China qingyuan innovation laboratory Quanzhou 362801China Fujian key laboratory of Advanced Manufacturing Technology of Specialty Chemicals Fuzhou UniversityFuzhou 350116China

Reversible chain transfer catalyzed polymerization(RTCP)is a practical and efficient process for the precise synthesis of polymers with special architecture by using simple phenols(2,4,6-trimethylphenol,TMP)or hydrocarbons(xanthene,XT)as efficient ***,alkyl iodide(R-1),which was gen erated from in situ bromine-iodine transformation of alkyl bromide(R-Br)with sodium iodide(Nal),was served as initiator to mediate RTCP with TMP or *** and other functional methacrylates,including GMA,DEAM,DMAEMA and BzMA,were successfully initiated by combining orga no catalysts and azo in itiators to yield polymers with low-polydispersity(M_(w)/M_(n)=1.1-1.5)and ideal mono mer conversions(50%-90%)at moderate *** over,3-armstar polymers were also obtained by this *** high chain-end fidelity of the obtained poly(methyl methacrylate)with iodine as chain-end group(PMMA-I)was confirmed by chain-extension *** en vironme ntally frie ndly initiators and orga no catalysts exhibit powerful polymerization properties toward RTCP,providing a sign ificant method to synthesize functional polymers.

关键词： Reversible chain transfer catalyzed polymerization Organocatalyst Halogen exchange

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High-efficiency and safe synthesis of tonalid via two Friedel-Crafts reactions in continuous-flow microreactors

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Chinese Journal of Chemical Engineering 2022年第12期52卷 126-135页

作者： Yang Han Yuanyuan Liu Shiwei Wang Xuehui Ge Xiaoda Wang Ting Qiu Engineering Research Center of Reactive Distillation Fujian Province Higher Education InstitutesCollege of Chemical EngineeringFuzhou UniversityFuzhou 350108China qingyuan innovation laboratory Quanzhou 362801China

Tonalid,an important fragrance ingredient with widespread applicatio n,was synthesized via two FriedelCrafts reactions,which were catalyzed by AlCl_(3).The traditional tonalid production was conducted in batch stirring tank reactors,suffering from low production capacity and the safety hazard of temperature *** solve these problems,the continuous-flow technologies were developed for the highefficiency and intrinsically safe synthesis of tonalid in *** AlCl_(3)was neatly homogenized in proper solvents by forming complex with reactant,which was a necessary step for the continuous synthesis in *** reaction conditions,including reactant molar ratio,catalyst concentration,temperature,and microchannel hydrodynamic diameter,were investigated for the two Friedel-Crafts reactions in micro *** optimized conditions,the yields of the two Friedel-Crafts reactions were 44.15%and 97.55%,*** comparison with the batch reactors,the reaction times of these two reactions could both be reduced by nearly two thirds in microreactors at the similar yield.

关键词： Microreactor Continuous synthesis Process intensification Tonalid Friedel-Crafts reaction

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