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Photoinduced transposed Paternò-Büchi reaction for effective synthesis of high-performance jet fuel

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Chinese Journal of Chemical Engineering 2024年第3期67卷 39-48页

作者： Jinxiu Hu Xianlong Liu Yi Liu Kang Xue chengxiang shi Xiangwen Zhang Li Wang Ji-Jun Zou Lun Pan Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic ***,we investigated the transposed Paternò-Büchi reaction of biomass cyclic ketone and cyclic alkene to synthesize a new kind of alkyl-substituted polycyclic hydrocarbon fuel with high energy density and good cryogenic *** triplet-energy-quenching results and phosphorescent emission spectra reveal the sensitization mechanism of the reaction,including photosensitizer excitation,triplettriplet energy transfer,cyclization,and relaxation,and the possible reaction path was revealed by the density functional theory(DFT)*** reaction conditions of photosensitizer type and addition,molar ratio of substrates,reaction temperature,and incident light intensity were optimized,with the target product yield achieving 65.5%.Moreover,the reaction dynamics of the reaction rate versus the light intensity are *** the hydrogenation-deoxygenation reaction,three fuels with a high density of 0.864-0.938 g·ml^(-1) and a low freezing point of<-55℃ are *** work provides a benign and effective approach to synthesize high-performance fuels.

关键词： High-energy-density fuel Transposed Patern-oeBüchi reaction Kinetics Bioenergy Photochemistry

Tandem hydroalkylation and deoxygenation of lignin-derived phenolics to synthesize high-density fuels

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Chinese Journal of Chemical Engineering 2024年第2期66卷 104-109页

作者： Rui Yu Zhensheng Shen Yanan Liu chengxiang shi Juncong Qu Lun Pan Zhenfeng Huang Xiangwen Zhan g Ji-Jun Zou Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Lignin is the most abundant naturally phenolic biomass,and the synthesis of high-performance renewable fuel from lignin has attracted significant *** propose the efficient synthesis of high-density fuels using simulated lignin cracked oil in tandem with hydroalkylation and deoxygenation ***,we investigated the reaction pathway for the hydroalkylation of phenol,which competes with the hydrodeoxygenation form *** then,we investigated the effects of metal catalyst types,the loading amount of metallic,acid dosage,and reactant ratio on the reaction *** phenol hydroalkylation and hydrodeoxygenation were balanced when 180℃ and 5 MPa H_(2)with the alkanes yield of 95%.By extending the substrate to other lignin-derived phenolics and simulated lignin cracked oil,we obtained the polycyclic alkane fuel with high density of 0.918 g·ml^(-1)and calorific value of41.2 MJ·L^(-1).Besides,the fuel has good low-temperature properties(viscosity of 9.3 mm^(2)·s^(-1)at 20℃ and freezing point below-55℃),which is expected to be used as jet *** work provides a promising way for the easy and green production of high-density fuel directly from real lignin oil.

关键词： High-density fuel Biofuel Hydrogenation Alkylation Lignin Phenolics

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吸热型纳米流体燃料研究进展

化工学报 2024年第4期75卷 1167-1182页

作者：申州洋薛康刘青史成香邹吉军张香文潘伦天津大学化工学院天津300072

吸热型纳米流体燃料是一种有潜力解决高超声速飞行器发动机过热问题的新型燃料。为探究吸热型纳米流体燃料的裂解性能,并为后续研究提供参考,首先介绍了纳米流体燃料的分散稳定性机理,并概述了其制备及提高稳定性的方法;其次,综述了吸... 详细信息

吸热型纳米流体燃料是一种有潜力解决高超声速飞行器发动机过热问题的新型燃料。为探究吸热型纳米流体燃料的裂解性能,并为后续研究提供参考,首先介绍了纳米流体燃料的分散稳定性机理,并概述了其制备及提高稳定性的方法;其次,综述了吸热型纳米流体燃料的裂解研究进展,从纳米添加剂、有机保护配体及反应机理和路径等多方面分析了影响裂解的关键因素;最后对吸热型纳米流体燃料的未来发展趋势提出展望。

关键词：燃料表面活性剂分散稳定性纳米粒子催化裂解催化机理

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Chiral pillar[n]arenes:Conformation inversion,material preparation and applications

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Chinese Chemical Letters 2022年第8期33卷 3613-3622页

作者： chengxiang shi Hui Li Xiaofeng shi Liang Zhao Hongdeng Qiu CAS Key Laboratory of Chemistry of Northwestern Plant Resources and Key Laboratory for Natural Medicine of Gansu Province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China Department of Gansu Provincial Cancer Hospital Institute of Materia MedicaLanzhou 730000China College of Chemistry Zhengzhou UniversityZhengzhou 450001China College of Chemistry and Chemical Engineering Gannan Normal UniversityGanzhou 341000China

Chiral pillar[n]arenes have shown great research value and application prospect in construction of chiral materials and chiral applications,due to their inherent planar chiral configurations,chiral recognition ability,easy modification and highly symmetric hydrophobic *** review systematically summarized the conformation inversion factors of planar chiral pillar[5]arenes(pR/p S),such as solvents,temperature,substituent size,alkyl chains,chiral and achiral guest *** firstly introduced the applications of chiral pillar[n]arenes for constructing chiral materials and pointed out that planar conformation inversion showed a great potential role in constructing chiral ***,we mainly concluded the chiral applications of chiral and planar chiral pillar[n]arenes like chiral enantiomer analysis by circular dichroism,electrochemistry or chiral fluorescence *** this review,we found that the inherent planar chiral conformation of chiral pillar[n]arenes have played a very important role in chiral field in the future.

关键词： Chiral pillar[n]arene Planar chiral configuration Chiral supramolecular materials Chiral separation and analysis Conformation inversion

Thixotropic composite hydrogels based on agarose and inorganic hybrid gellants

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Chinese Journal of Chemical Engineering 2023年第2期54卷 240-247页

作者： Hongzhi Zhang Huiyan Guo Yang Liu chengxiang shi Lun Pan Xiangwen Zhang Ji-Jun Zou Key Laboratory for Advanced Fuel and Chemical Propellant of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Water can be used as oxidant in conjunction with metal particles to form metal-water propellant to increase the energy of *** this application,water needs to be stored in form of solid and capable of becoming liquid when *** and thixotropic hydrogel has good potential as water-retaining material and oxidant of metal-based *** this study,we prepared organic/inorganic composite hydrogels by combining inorganic gellants hectorite and fumed silica with organic gellant agarose,*** total content of the gellants can be reduced to less than 2%by adding *** influence of agarose on water content,phase transition temperature,centrifugal stability and other basic physical properties of composite hydrogels were *** results show that the composite hydrogels have better thixotropy and stability than pure inorganic hydrogels,and the gel-sol transformation can be realized by applying shear force or heating to the phase transition *** composite hydrogels have good shear thinning ability and improved mechanical *** silica/agarose hydrogels have better physical stability,while the thixotropy and shear thinning ability of hectorite/agarose hydrogels are better.

关键词： Composite hydrogels Organic gellant Inorganic gellant Rheological properties

Conversion of lignin oil and hemicellulose derivative into high-density jet fuel

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Journal of Energy Chemistry 2023年第2期77卷 452-460,I0012页

作者： Sichao Yang chengxiang shi Zhensheng Shen Lun Pan Zhenfeng Huang Xiangwen Zhang Ji-Jun Zou Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Synthesizing high-density fuel from lignocellulose can not only achieve green and low-carbon development,but also expand the feedstock source of hydrocarbon ***,we reported a route of producing high-density fuel from lignin oil and hemicellulose derivative cyclopentanol through alkylation and hydrodeoxygenation,HY with SiO_(2)/Al_(2)O_(3) molar ratio of 5.3 was screened as the alkylation catalyst in the reaction of model phenolic compounds and mixtures,and the reaction conditions were optimized to achieve conversion of phenolic compounds higher than 87%and selectivity of bicyclic and tricyclic products higher than 99%.Then two phenolic pools simulating the composition of two typic lignin oils were studied to validate the alkylation and analyze the competition mechanism of phenolic compounds in mixture ***,real lignin oil from depolymerized of beech powder was tested,and notably80%of phenolic monomers in the oil were converted into fuel *** hydrodeoxygenation,the alkylated product was converted to fuel blend with a density of 0.91 g/mL at 20℃and a freezing point lower than-60℃,very promising as high density *** work provides a facile and energyefficient way of synthesizing high-performance jet fuel directly from lignocellulosic derivatives,which decreases processing energy consumption and improve the utilization rate of feedstock.

关键词： High-density fuel Biofuel Lignin oil Alkylation Hydrodeoxygenation

Metal-oxoacid-mediated oxyhydroxide with proton acceptor to break adsorption energy scaling relation for efficient oxygen evolution

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Journal of Energy Chemistry 2023年第5期80卷 594-602,I0013页

作者： Rongrong Zhang Beibei Guo Lun Pan Zhen-Feng Huang chengxiang shi Xiangwen Zhang Ji-Jun Zou Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207FujianChina Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Metal oxyhydroxides(MOOH)generated from irreversible reconstructions of transition metal compounds are intrinsic active species for oxygen evolution reaction,whose activities are still constrained by sluggish deprotonation kinetics and inherent adsorption energy scaling ***,we construct a tunable proton acceptor(TPA)on oxyhydroxides by in-situ reconstruction of metal oxoacids such as NiC2O4to accelerate deprotonation and break adsorption energy scaling relations during *** modified C_(2)O_(4)^(2-)as a TPA can easily extract H of*OH(forming*HC2O4intermediate)and then promote deprotonation by the transmitted hydrogen bond with*OOH along conjugated(H...)O=C-O(-H)*** a result,Ni OOH-C2O4shows non-concerted proton-electron transfer and improved deprotonation rate,and delivers a good OER activity(270 mV@10 mA cm-2).The conjugate acidity coefficient(pKa)of the modified oxoacid group can be a descriptor for TPA *** TPA strategy can be universally applied to Co-,Fe-,and Ni-based oxyhydroxides to facilitate OER efficiency.

关键词： Electrocatalysis Metal oxyhydroxide Oxoacid group Tunable proton acceptor Oxygen evolution reaction

Framework Zr Stabilized PtSn/Zr-MCM-41 as a Promising Catalyst for Non-oxidative Ethane Dehydrogenation

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Chinese Journal of Chemistry 2022年第8期40卷 918-924页

作者： Jisheng Xu chengxiang shi Shuguang Zhang Qiancheng Zheng Lun Pan Xiangwen Zhang Ji-Jun Zou Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Zhejiang Institute of Tianjin University NingboZhejiang315201China

Non-oxidative ethane dehydrogenation is a promising route to produce ***,PtSn supported catalysts were investigated to achieve better ethane dehydrogenation performance by introduction of different Zr promoters,i.e.,framework Zr and ZrO_(2),to mesoporous ***-situ XRD,TEM and CO chemisorption show that aggregation of metal particles and phase segregation of Pt_(3)Sn to Pt and PtSn_(3) at high temperature occur for PtSn/M,leading to bad ethane dehydrogenation *** interaction be-tween ZrO_(2) and PtSn species,as proved by XPS,results in restrained metal particles,which promotes the initial ***,Pt phase generated on surface is disadvantageous for the desorption of produced ethene as indicated by CO-IR and C_(3)H_(6)-TPD,and pyridine-IR and NH_(3)-TPD indicate strong acidity *** deactivate the catalyst rapidly by deep dehydrogenation and *** interaction between PtSn species and Si-O-Zr with much weaker acidity is formed when framework Zr is incorporated into MCM-41,which benefits the dispersion of metal particles,formation of Pt_(3)Sn/Pt species and stabilization of metal species from phase *** initial ethane conversion and ethene selectivity of ca.99%were achieved for the optimal PtSn/ZrM,which is more coking-tolerant and stable by generating graphitic carbon mainly on support instead of active metals.

关键词： Alkanes Dehydrogenation Platinum Framework heteroatoms Metal-support interaction

Chiral phenethylamine synergistic tricarboxylic acid modified β-cyclodextrin immobilized on porous silica for enantioseparation

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Chinese Chemical Letters 2023年第3期34卷 162-165页

作者： Hui Li Xiaoping Wang chengxiang shi Liang Zhao Zuguang Li Hongdeng Qiu CAS Key Laboratory of Chemistry of Northwestern Plant Resources and Key Laboratory for Natural Medicine of Gansu Province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014China

In this work, a series of chiral phenethylamine synergistic tricarboxylic acid modified β-cyclodextrin bonded stationary phase for high performance liquid chromatography(HPLC) were synthesized via a simple one-pot synthesis approach. Various racemates(aryl alcohols, flavanones, triazoles, benzoin, etc.) were well separated on the tricarboxylic acid modified chiral stationary phases in both normal and reversed modes with good reproducibility and stability, and the influence of mobile phase composition on resolution(R_(s)) were deeply investigated. The RSD values of Rsfor repeatability and column-to-column were below 1.28% and 3.05%, respectively. Hence, the fabrication of tricarboxylic acid modified chiral stationary phase(CSPs) is a new efficient strategy to improve the application of β-cyclodextrin as CSPs in the field of chromatography.

关键词： Tricarboxylic acid β-cyclodextrin Chiral stationary phases Enantioseparation One-pot strategy