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Continuous microflow visible-light photocatalytic N-formylation of piperidine and its kinetic study

Chinese chemical Letters 2024年第1期35卷 285-289页

作者： Yangyang Xu Fang Zhao Xuhong Guo State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China International Joint Research Center of Green Energy Chemical Engineering Shanghai 200237China

N-formylation of amines,a class of synthetically important reactions,is typically conducted using metal catalysts that are relatively expensive or not readily available and usually needs harsh conditions to increase the reaction ***,an efficient continuous microflow strategy was developed for the gas-liquid visible-light photocatalytic N-formylation of piperidine,which achieved a reaction yield of 82.97%and a selectivity of>99%at 12 min using cheap organic dye photocatalyst under mild reaction *** influence of essential parameters,including light intensity,temperature and equivalents of the gas,additive and photocatalyst,on the reaction yield was systematically ***,kinetic investigations were conducted,exhibiting the dependence of reaction rate and equilibrium yield of N-formylpiperidine on light intensity,temperature and photocatalyst *** microflow photocatalytic approach established in this work,which realized a markedly higher space-time yield than the conventional batch method(37.9 vs.0.212 mmol h-1 L-1),paves the way for the continuous,green and efficient synthesis of N-formamides.

关键词： Microflow Visible-light photocatalysis N-Formylation Piperidine Kinetics

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Reconstruction of Cu-ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol

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Frontiers of chemical Science and engineering 2023年第9期17卷 1311-1319页

作者： Fan Sun Huijiang Huang Wei Liu Lu Wang Yan Xu Yujun Zhao Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

A reconstructed Cu-ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,*** to the characterization results of the fresh Cu-ZnO and reconstructed Cu-ZnO,three different forms of ZnO were suggested to be presented on the catalysts:ZnO having strong interaction with Cu species,ZnO that weakly interacted with Cu species and isolated *** first form of ZnO was believed to be beneficial to the formation of efficient active site Cu^(+),while the latter two forms of ZnO took the main responsibility for the deactivation of Cu-ZnO catalysts in the liquid-phase hydrogenation of *** reconstruction of the Cu-ZnO catalyst by the organic acid treatment method resulted in a new Cu-ZnO catalyst with more Cu^(+)and less ZnO species that leads to ***,the deactivation mechanism of Cu-ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed:the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the *** results provided meaningful instructions for designing highly efficient Cu-Zn catalysts for similar ester hydrogenation systems.

关键词： liquid phase hydgonenation Cu-ZnO deactivation mechanism 1,4-butanediol diester

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Controllable photooxidation of 1-phenylethanol integrated with hydrogen evolution by a polyoxometalate/ZnIn_(2)S_(4)/WO_(3)catalytic system

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Nano Research 2025年第4期18卷 116-124页

作者： Jiaxin Yang Yongkang Liu Yun Qin Zhenheng Diao Yuanyuan Dong Hongjin Lv School of Chemical Engineering Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectric/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

The photocatalytic oxidation of 1-phenylethanol coupling with hydrogen evolution represents a promising strategy for the full utilization of the photogenerated electrons and holes to accomplish the maximum conversion of solar energy into chemical *** date,however,the controllable of reaction path and product distribution has yet not to be ***,we report an efficient coupled catalytic system composed of ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction and Ni-containing polyoxometalate([Ni_(4)(H_(2)O)_(2)(PW_(9)O_(34))_(2)]^(10-)(Ni_(4)P_(2))),which exhibited excellent photocatalytic activities towards the oxidation valorization of 1-phenylethanol coupling with hydrogen *** addition of Ni_(4)P_(2)can efficiently control the product ***,1-phenylethanol was preferentially converted to pinacol(86.0% selectivity)via C-C coupling over ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction accompanied by hydrogen production(202.4μmol),whereas it would be converted to acetophenone(93.8% selectivity)by photogenerated holes with concomitant hydrogen formation(183.1μmol)over the coupled Ni_(4)P_(2)/ZnIn_(2)S_(4)/WO_(3) catalytic *** studies revealed that the hydrogen evolution cocatalyst Ni4P2,with its excellent electron storage capacity,can compete with the oxidation product acetophenone for electrons,and thus its addition can significantly inhibit the reduction of acetophenone,resulting in the inability to generate the coupling product pinacol.

关键词： S-scheme heterojunction ZnIn_(2)S_(4) polyoxometalates dehydrocoupling hydrogen evolution photocatalysis

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Bottlebrush Random Copolymers at Oil-Oil Interfaces

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Chinese Journal of Chemistry 2025年第2期43卷 139-145页

作者： Yaxin Wang Yunhui Wen Yuzheng Luo Shuailong Li Jiaqiu Luo Shaowei Shi State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing100029 China

Oil-in-oil nonaqueous emulsions are of great interest for developing emulsion-templated polymers and encapsulation systems that are incompatible with water-sensitive ***-made amphiphilic block copolymers are by far the most efficient stabilizers for oil-in-oil emulsions while less attention is given to copolymers with more complex ***,we report the stabilization of DMSO-silicone oil interface by bottlebrush random copolymers(BRCPs)containing norbornene backbones with densely grafted poly(methyl methacrylate)(PMMA)and polystyrene(PS)side *** assembly kinetics of BRCPs at the DMSO-silicone oil interface can be divided into three processes,including diffusion,reconfiguration and reorganization,and can be varied by tuning the degree of polymerization of the backbone(NB).Due to the high efficiency of BRCPs in reducing the interfacial tension,when using BRCPs as stabilizers,stable silicone oil-in-DMSO traditional emulsions and high internal phase emulsions(HIPEs)can be successfully obtained,while no stable emulsions can be achieved with linear PMMA-b-PS serving as the *** study,for the first time,underscores the great potential of amphiphilic bottlebrush copolymers in preparing oil-in-oil *** the advances in polymerization strategy,a broad variety of amphiphilic bottlebrush copolymers are expected to be synthesized and applied in the stabilization of nonaqueous biphasic systems.

关键词： Bottlebrush copolymers Oil-oil interfaces|Emulsions Surfactants Assembly dynamics

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Flexible Organic Crystal with Two-Dimensional Elastic Bending and Recoverable Plastic Twisting for Circularly Polarized Luminescence

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CCS Chemistry 2024年第6期6卷 1439-1447页

作者： Wenjie Kuang Bo Jing Songgu Wu Junbo Gong State Key Laboratory of Chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072 Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072

Multidimensional mechanical flexible organic crystals with tunable optoelectronic properties hold significant promise for practical application in complicated environmental ***,based on a newly designed“flexible”Schiff base small molecule with chirality,we presented a compatibly bendable and twistable organic single crystal with circularly polarized luminescence for the first ***,the twodimensional elastic bending of the chiral crystal was realized at both room and liquid nitrogen temperatures,along with recoverable plastic twisting at room ***,circular dichroism and circularly polarized luminescence spectroscopy were employed to characterize the chiral enantiomer in solution and the solid *** design strategy provides a new perspective for the future construction of chiroptical flexible crystal materials.

关键词： organic crystal multidimensional flexibility circularly polarized luminescence low-temperature resistance

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Nano-silica modified lightweight and high-toughness carbon fiber/phenolic ablator with excellent thermal insulation and ablation performance

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Defence technology（防务技术） 2024年第1期31卷 192-199页

作者： Wenjie Xu Wenda Song Xianfeng Jia Cheng Ma Jitong Wang Wenming Qiao Licheng Ling State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering and Materials Changzhou Institute of TechnologyChangzhou 213032China Key Laboratory of Specially Functional Polymeric Materials and Related Technology(Ministry of Education) School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China

Lightweight and high-toughness carbon fiber/phenolic ablator(CFPA)is required as the Thermal Protection System(TPS)material of aerospace vehicles for next-generation space *** improve the ablative properties,silica sol with good particle size distribution prepared using tetramethoxysilane(TMOS)was blended with natural rubber latex and deposited onto carbon fiber felt,which was then integrated with phenolic aerogel matrix,introducing nano-silica into the framework of *** modified CFPA with a low density of 0.28—0.31 g/cm3exhibits strain-in-fracture as high as 31.2%and thermal conductivity as low as 0.054 W/(m·K).Furthermore,a trace amount of nano-silica could effectively protect CFPA from erosion of oxidizing atmosphere in different high-temperature *** oxyacetylene ablation test of 3000°C for 20 s shows a mass ablation rate of 0.0225 g/s,a linear ablation rate of 0.209 mm/s for the modified CFPA,which are 9.64%and 24.82%lower than the unmodified ***,the long-time butane ablation test of 1200°C for 200 s shows an insignificant recession with mass and linear ablation rate of 0.079 g/s and 0.039 mm/s,16.84%and 13.33%lower than the unmodified ***,the fixed thermocouple in the test also demonstrates a good thermal insulation performance with a low peak back-face temperature of 207.7°C,12.25%lower than the unmodified ***,the nano-silica modified CFPA with excellent overall performance presents promising prospects in high-temperature aerospace applications.

关键词： Nano-silica Carbonfiber Phenolic aerogel Insulation Ablation

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Multiple exciton generation effect in photocatalytic overall water splitting

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Science China Chemistry 2024年第2期67卷 424-425页

作者： Xiaolei Guo Ji-Jun Zou Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

This highlight is based on recent research published in Nature Energy by Li and co-workers [1] from Northwestern Polytechnology University, reporting an exceeding 100% internal quantum efficiency(IQE) in photocatalytic overall water splitting. This breakthrough promises a bright future for efficient photocatalyst design by utilizing the multiple exciton effect(MEG).

关键词： splitting effect utilizing

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Yolk-shell FeCu/NC electrocatalyst boosting high-performance zinc-air battery

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Nano Research 2024年第9期17卷 7918-7925页

作者： Chen Liang Tianyu Zhang Shilun Sun Aijuan Han Zenghui Qiu Haijun Xu Junfeng Liu State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China College of Mathematics&Physics Beijing University of Chemical TechnologyBeijing 100029China Beijing Bioprocess Key Laboratory Beijing University of Chemical TechnologyBeijing 100029China

Iron-nitrogen-carbon single-atom catalysts(Fe-N-C SACs)are widely acknowledged for their effective oxygen reduction activity,however,their activity requires further ***,additional structural optimization is necessary to enhance mass transport and achieve higher power density in practical ***,using ZIF-8 as a template,we synthesized yolk-shell catalysts featuring complex sites of Fe single atoms and Cu nanoclusters(y-FeCu/NC)via partial etching and liquid-phase *** synthesized y-FeCu/NC catalyst exhibits high specific surface area and mesoporous *** with the advantages of highly active sites and yolk-shell structure,the y-FeCu/NC catalyst demonstrated outstanding catalytic performance in the oxygen reduction reaction,achieving a half-wave potential(E_(1/2))of 0.97 V in 0.1 M *** a practical energy device,Zn-air battery(ZAB)assembled with y-FeCu/NC catalyst achieved a remarkable power density of 356.3 mW·cm^(-2),representing an improvement of approximately 28.5%compared to its solid FeCu/NC ***,it showcased impressive stability,surpassing all control samples.

关键词： atomic Fe-N4 sites Cu nanoclusters yolk-shell structure oxygen reduction reaction zinc-air battery

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Highly Sensitive Ethanol Gas Sensor Based on Ag Nanoparticles Decorated In_(2)O_(3)

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chemical Research in Chinese Universities 2024年第6期40卷 1033-1040页

作者： ZHANG Susu ZHANG Meng GUO Ying State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029P.R.China

Ag nanoparticle decorated In_(2)O_(3) composites for high sensitivity and high selectivity detection of ethanol were prepared by hydrothermal and annealing *** effects of Ag content on the sensing properties of Ag decorated In_(2)O_(3) sensors were also *** was found that all Ag decorated In_(2)O_(3) sensors exhibited better sensing performance in terms of sensitivity and selectivity compared to pure In_(2)O_(3) *** optimizing the addition amount of Ag,the 7%-Ag/In_(2)O_(3) sensor showed the highest response to ethanol (35.6 vs.100 ppm,ppm=parts per million);which was about seven times higher than that of the pure In_(2)O_(3) sensor at 270 ℃.The improved performance of the Ag-In_(2)O_(3) composite sensor can be attributed to the catalytic effect of silver and the Schottky barrier formed at the Ag-In_(2)O_(3) interface.

关键词： Ag In_(2)O_(3) Schottky barrier Ethanol Sensor

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Rhodium complex-anchored and supramolecular polymer-grafted CdS nanoflower for enhanced photosynthesis of H_(2)O_(2) and photobiocatalytic C–H bond oxyfunctionalization

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Frontiers of chemical Science and engineering 2024年第10期18卷 73-82页

作者： Hongwei Jia Xiaoyang Yue Yuying Hou Fei Huang Cuiyao Cao Feifei Jia Guanhua Liu Xiaobing Zheng Yunting Liu Yanjun Jiang School of Chemical Engineering and Technology Hebei University of TechnologyTianjin 300401China National-Local Joint Engineering Laboratory for Energy Conversion in Chemical Process Integration and Resources Utilization School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300401China

Unspecific peroxygenases exhibit high activity for the selective oxyfunctionalization of inert C(sp3)–H bonds using only H_(2)O_(2) as a clean oxidant,while also exhibiting sensitivity to H_(2)O_(2) ***-based semiconductors are promising for the photosynthesis of H_(2)O_(2) owing to their adequately negative potential for oxygen reduction reaction via a proton-coupled electron transfer process,however,they suffer from fast H_(2)O_(2) decomposition on the surface of pristine ***,[Cp*Rh(bpy)H_(2)O]2+,a highly selective proton-coupled electron transfer catalyst,was anchored onto a supramolecular polymer-grafted CdS nanoflower to construct an efficient integrated photocatalyst for generating H_(2)O_(2),mitigating the surface issue of pristine CdS,increasing light absorption,accelerating photonic carrier separation,and enhancing oxygen reduction reaction selectivity to H_(2)O_(2).This photocatalyst promoted the light driven H_(2)O_(2) generation rate up to 1345μmol·L^(-1)·g^(-1)·h^(-1),which was 2.4 times that of pristine *** constructed heterojunction photocatalyst could supply H_(2)O_(2) in situ for nonspecific peroxygenases to catalyze the C–H oxyfunctionalization of ethylbenzene,achieving a yield of 81%and an ee value of 99%under optimum conditions.A wide range of substrates were converted to the corresponding chiral alcohols using this photo-enzyme catalytic system,achieving the corresponding chiral alcohols in good yield(51%–88%)and excellent enantioselectivity(90%–99%ee).

关键词： cadmium sulfide unspecific peroxygenases photobiocatalysis hydrogen peroxide oxyfunctionalization

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