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Influence of Ca/P ratio on the catalytic performance of hydroxyapatite for decarboxylation of itaconic acid to methacrylic acid

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Chinese Journal of chemical engineering 2023年第1期53卷 402-408页

作者： Shutong Pang Hualiang An Xinqiang Zhao Yanji Wang Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

Methacrylic acid,an important organic chemical,is commercially manufactured starting from fossil *** decarboxylation of itaconic acid derived for biomass is a green route to the synthesis of methacrylic *** view of the problems existing in the researches on this route such as use of noble metal catalyst,harsh reaction conditions and low desired-product yield,we prepared a series of hydroxyapatite catalysts with different Ca/P molar ratios and evaluated their catalytic *** results showed that the hydroxyapatite catalyst with a Ca/P molar ratio of 1.58 had the best catalytic *** highest yield of MAA up to 61.2%was achieved with basically complete conversion of itaconic acid under the suitable reaction conditions of 1 equivalent of NaOH,2 MPa of N_(2),250℃,and 2 *** this basis,a reaction network for the decarboxylation of itaconic acid to methacrylic acid catalyzed by hydroxyapatite was *** the aid of catalyst characterization using X-ray powder diffraction,NH3/CO2 temperature-programmed desorption,N_(2)physisorption,inductively coupled plasma optical emission spectrometry,and scanning electron microscopy,we found that the distribution of surface acid sites and basic sites,crystal growth orientation,texture properties and morphology of hydroxyapatite varied with the Ca/P molar ***,the change of the crystal growth orientation and its influence on the surface acidity and alkalinity were clarified.

关键词： Biomass-derived itaconic acid Methacrylic acid Hydroxyapatite catalyst Ca/P ratio Decarboxylation reaction

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Coupled Cu doping and Z-scheme heterojunction for synergistically enhanced tetracycline photodegradation

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Nano Research 2024年第7期17卷 5937-5948页

作者： Huidong Shen Chunming Yang Song Hong Leiduan Hao Liang Xu Alex W.Robertson Zhenyu Sun Country State Key Laboratory of Organic-Inorganic Composites College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China Shaanxi Key Laboratory of Chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China Department of Physics University of WarwickCoventry CV 47ALUK

Semiconductor-based photocatalysis by utilizing solar energy for sustainable organic pollutant elimination has been a promising tactic to alleviate environmental ***,the development of robust and efficient photocatalysts to degrade organic pollutants still faces major challenges because of insufficient charge *** we design and fabricate a heterojunction consisting of copper,carbon-modified TiO_(2),and sulfur-doped g-C_(3)N_(4)nanosheets(i.e.,S-C_(3)N_(4)/Cu/C-TiO_(2)).The heterostructure affords a remarkable synergistic photocatalysis for tetracycline hydrochloride degradation,achieving an 82.6%removal efficiency within 30 min under visible light irradiation,about 15.4 and 7.3 times higher than that of S-C_(3)N_(4)and C-TiO_(2),*** superior performance is attributed to the synergy between Cu doping and the Z-scheme heterojunction,which not only enhances the interfacial electric field effect,facilitating charge separation,but also boosts the redox *** charge carrier transfer between Cu/C-TiO_(2)and S-C_(3)N_(4)follows a Z-scheme,as verified by trapping experiments,electron spin-resonance spectroscopy,and density functional theory ***,the tetracycline hydrochloride degradation pathways are enunciated by liquid chromatograph mass spectrometry *** work provides an effective approach for constructing high-performance photocatalysts that have potential in environmental remediation.

关键词： photocatalysis Cu doping Z-scheme heterojunction electrons and holes separation tetracycline degradation

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A Mn-porphyrinic metal–organic framework immobilizing glucose oxidase for combined photodynamic/chemodynamic/starvation therapy

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Tungsten 2025年第1期7卷 183-194页

作者： Xin-Ran Sun Hao-Ming Yuan Guo-Da Zhang Chao Wang Shu-Juan Sun Peng-Fei Shi Shandong Provincial Key Laboratory of Detection Technology for Tumor Markers School of Chemistry and Chemical Engineering Linyi University

The combination of photodynamic therapy（PDT） and chemodynamic therapy（CDT） in tumor treatment has attracted considerable ***,tumor hypoxia and glutathione（GSH） overproduction in the tumor tissue restricted the progress of their ***,a Mn-porphyrinic metal-organic framework（Mn-TCPP） was constructed by the one-pot method and further used for immobilizing glucose oxidase（GOx） to obtain GOx@*** would rapidly exhaust endogenous glucose into hydrogen peroxide（H2O2） and gluconic acid,thus shutting off the energy supply of tumor cells for starvation ***-TCPP catalyzed H2O2to produce oxygen,regulating the hypoxic tumor microenvironment and in turn improving1O2generation under laser ***,Mn-TCPP can reduce reactive oxygen species consumption owing to the redox reaction between Mn3+and GSH,thus greatly enhancing ***,benefiting from GOx-mediated starvation therapy,Mn2+produced by Mn3+reduction can react with sufficient intracellular H2O2to generate ·OH with high cytotoxicity through a Fenton-like *** treatment by GOx@Mn-TCPP under laser irradiation in vitro,the cell viability of 4T1 and A549 tumor cells reached to 20%,reflecting GOx@Mn-TCPP could give full play to the advantages of PDT/CDT/starvation *** results in vivo demonstrated that GOx@Mn-TCPP mediated synergistic cascade therapy could significantly inhibit tumor growth and improve the therapeutic effect.

关键词： Metal-organic frameworks Immobilizing enzyme Photodynamic therapy Chemodynamic therapy Starvation therapy

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Design and control of fraction cutting for the separation of mixed alcohols from the Fischer-Tropsch aqueous by-products

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Chinese Journal of chemical engineering 2022年第10期50卷 143-154页

作者： Renren Zhang Yang Huang Kaitian Zheng Chunjian Xu School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringChemical Engineering Research CenterTianjin UniversityTianjin 300072China

Since the minimum-boiling azeotropes of C2-C8 alcohols with water and high-water content(up to 95%(mass))in the Fischer-Tropsch aqueous by-products,the separation is energy-intensive and *** energy-saving strategy for the complete separation of the Fischer-Tropsch aqueous by-products has received massive attention in recent *** this study,a stripper-sidestream decanter process is proposed by exploiting homogeneous azeotropes(C2-C3 alcohols-water)and heterogeneous azeotropes(C4-C8 alcohols-water).The introduction of the stripping column for pre-dehydration avoids the revaporization of the mixture,and energy carried by the overhead vapor is conserved instead of being removed in a *** precise fraction cutting of C1-C3 alcohol-water mixture,C4-C8 alcohols,and water is realized by the sidestream distillation *** C4-C8 alcohols rich mixture withdrawn from the sidestream flows into the decanter to break the distillation boundary,where the organic phase returns to the sidestream distillation column to obtain the dehydrated C4-C8 alcohols,and the aqueous phase enters the stripping ***-state optimization based on total annual cost(TAC)minimization shows that the stripper-sidestream decanter process reduces TAC by 17.00%and saves energy by 21.27%compared with the conventional three-column distillation ***,a control structure of the process is established,and dynamic simulations show that the control structure combining a differential controller with a low-selector exhibits robust co *** study provides a novel design scheme and deepens the insights into the efficient separation of aqueous by-products of the Fischer-Tropsch synthesis.

关键词： Fischer–Tropsch synthesis Mixed alcohols Azeotrope Separation Simulation Control

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Polygonal mesopores microflower catalysts for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene to 2-nitro-4-methylsulfonylbenzoic acid in a continuous-flow microreactor

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Chinese Journal of chemical engineering 2024年第9期73卷 212-221页

作者： Jianzhi Wang Xugen Li Cheng Zhang Yuan Pu Jiawu Liu Jie Liu Yanping Liu Xiao Lin Faquan Yu Key Laboratory for Green Chemical Process of Ministry of Education Hubei Key Laboratory for Novel Reactor and Green Chemistry TechnologyHubei Engineering Research Center for Advanced Fine ChemicalsSchool of Chemical Engineering and PharmacyWuhan Institute of TechnologyWuhan 430073China

The development of efficient systems for the catalytic oxidation of 2-nitro-4-methylsulfonyltoluene(NMST)to 2-nitro-4-methylsulfonyl benzoic acid(NMSBA)with atmospheric air or molecular oxygen in alkaline medium presents a significant challenge for the chemical ***,we report the synthesis of FeOOH/Fe_(3)O_(4)/metal-organic framework(MOF)polygonal mesopores microflower templated from a MIL-88B(Fe)at room temperature,which exposes polygonal mesopores with atomistic edge steps and lattice *** obtained FeOOH/Fe_(3)O_(4)/MOF catalyst was adsorbed onto glass beads and then introduced into the microchannel *** the alkaline environment,oxygen was used as oxidant to catalyze the oxidation of NMST to NMSBA,showing impressive *** sustainable system utilizes oxygen as a clean oxidant in an inexpensive and environmentally friendly NaOH/methanol *** position and type of substituent critically affect the ***,this sustainable protocol enabled gram-scale preparation of carboxylic acid and benzyl alcohol derivatives with high ***,the reactions can be conducted in a pressure reactor,which can conserve oxygen and prevent solvent ***,compared with the traditional batch reactor,the self-built microchannel reactor can accelerate the reaction rate,shorten the reaction time,and enhance the selectivity of catalytic oxidation *** approach contributes to environmental protection and holds potential for industrial applications.

关键词： 2-nitro-4-methylsulfonylbenzoic 2-nitro-4-methylsulfonyltoluene FeOOH/Fe3O4/MOF Catalyst Microreactor Oxidation

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Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China State Key Laboratory of Petroleum Molecular and Process Engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

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Simplified p-i-n Perovskite Solar Cells with a Multifunctional Polyfullerene Electron Transporter

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Chinese Journal of Polymer Science 2024年第8期42卷 1060-1066页

作者： Fei-Fei Wang Tian-Xiao Liu Ze-Wei Cui Ling-Yuan Wang Yun-Jie Dou Xiao-Yu Shi Si-Wei Luo Xiao-Dong Hu Zhi-Jun Ren Yang-Yang Liu Yu Zhao Shang-Shang Chen State Key Laboratory of Coordination Chemistry MOE Key Laboratory of High Performance Polymer Materials&TechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 21003China

In prevailing p-i-n perovskite solar cells(PSCs),solution-processible fullerene molecules are widely used as electron-transporting layers(ETLs)but they typically suffer from poor uniformity and undesirable stability ***,a separate bathocuproine(BCP)layer is needed to block hole tran sfer,increasing fabrication complexity and ***,we address these limitations by develo ping a novel polymeric ETL(named PF BCP)synthesized by polymerizing C_(60)with *** innovative material achieves both efficient electron transport and hole blocking,while its excellent uniformity minimizes interface recombination and enhances ***,our blade-coated PSCs utilizing PFBCP achieve a high power conversion efficiency exceeding 22%and retain 91%of initial efficiency after 1200 h of light *** development not only paves the way for commercially viable PSCs but also opens avenues for future ETL design to realize even more efficient and stable PSCs.

关键词： Polyfullerene Perovskite solar cells Electron transporter Stability

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Design and mechanism of agglomeration of aspirin crystals in pure solvents

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Particuology 2023年第11期82卷 146-156页

作者： Lihong Jia Degui Wu Pingping Cui Ling Zhou Qiuxiang Yin School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China Tianjin Key Laboratory of Modern Drug Delivery and High Efficiency Tianjin300072China

Agglomeration with improved flowability for platy crystals is desirable in pharmaceutical downstream processing. The formation of agglomerates in pure solvents without the aid of bridging liquids is a convenient and low-cost method compared with complex spherical crystallization. In this work, the adhesion free energies between aspirin crystals in six solvents were calculated using Lifshitz-van der Waals acid-base theory to screen suitable solvents for agglomeration. The maximum stirring rate for agglomeration was determined by adhesion forces and dispersion forces. Then the agglomerates of plate-shaped aspirin were successfully prepared in acetone, methanol, ethanol, 2-propanol, and ethylene glycol without additives by simple cooling crystallization. The interactions between solvent and crystal surfaces were also used to explain the outcomes. A feasible mechanism for the agglomeration process of platy crystals was elucidated, involving the adhesion of dominant crystal facets at the beginning. The effect of stirring rate, cooling rate, and initial supersaturation on agglomeration degree and particle size of aspirin agglomerates were studied. The obtained aspirin agglomerates under the optimal conditions exhibited a uniform particle size distribution, a high agglomeration degree, and superior flowability.

关键词： Agglomeration Platy crystal Aspirin Adhesion force

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Synthetic Features and Mechanism for the Preparation of Vinyl Chloride-co-Butyl Acrylate-co-Vinyl Acetate Terpolymer via Precipitation Polymerization

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Chinese Journal of Polymer Science 2023年第11期41卷 1714-1724,I0006页

作者： Chang-Tong Song Xian-Hong Zhang Dong Chen Yu-Hong Ma Wan-Tai Yang State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China College of Material Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China

Without any type of su rfactant or dispersing agent,precipitation polymerization has great superiorities in both polymer synthesis and *** the present work,the polymerization of vinyl chloride(VC),n-butyl acrylate(BA),and vinyl acetate(VAc)are conducted in the precipitation polymerization system and series of their random terpolymers poly(vinyl chloride-co-n-butyl acrylate-co-vinyl acetate)(PCBV)are synthesized *** effects of various polymerization conditions,including solvent polarity,temperature,initiator concentration,and monomer feed ratios on the polymerization kinetics,number-average molecular weight(M_(n)),and terpolymer composition are investigated *** solvent and the monomer feed ratio are crucial factors not only for the polymer morphology,but also for the reaction *** the non-polar solvent such as n-hexane,the PCBV displays particle morphology when the composition of BA ratio lower than 10 wt%.Otherwise,the PCBV forms a uniform polymer phase and precipitates out from the *** the polar solvent,e.g.,dimethyl carbonate(DMC)and ethanol,the PCBV polymer maintains a slurry state either in low or in high monomer feed ***,VC based ternary copolymer that obtained in n-hexane has much lower M_(n)(<20 kDa)and much higher BA units mass fraction(>40 wt%)compared with emulsion and suspension ***,the terpolymer can be easily sepa rated by simple centrifugation.

关键词： Precipitation polymerization Copolymerization Vinyl chloride Low molecular weight

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Electrostatically driven kinetic inverse CO_(2)/C_(2)H_(2) separation in LTA-type zeolites

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Chinese Journal of Structural Chemistry 2024年第10期43卷 27-34页

作者： Yongheng Ren Yang Chen Hongwei Chen Lu Zhang Jiangfeng Yang Qi Shi Lin-Bing Sun Jinping Li Libo Li College of Chemical Engineering and Technology State Key Laboratory of Clean and Efficient Coal UtilizationTaiyuan University of TechnologyTaiyuan030024China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

The identical molecular size and similar physical properties of carbon dioxide(CO_(2))and acetylene(C_(2)H_(2))make their adsorptive separation extremely challenging to achieve with most *** on the separation of CO_(2)and C_(2)H_(2)mixtures by zeolites are even rarer with the mechanism of adsorptive separation requiring further *** this paper,we report that ion modulation of zeolite 5A promotes the difference in kinetic diffusion of CO_(2)and C_(2)H_(2),realizing the inverse separation of zeolite from selective adsorption of C_(2)H_(2)to selective adsorption of CO_(2).Creating a compact pore space restricting the orientation of gas molecules enables charge *** positive electrostatic potential at the pore openings was utilized to hinder the diffusion of C_(2)H_(2)between the cages while ensuring the transfer of CO_(2),increasing their diffusion differences in pore channels and leading to the CO_(2)/C_(2)H_(2)kinetic selectivity of *** canonical Monte Carlo(GCMC)simulation demon-strates that the CO_(2)distribution in K-5A-βis significantly higher than that of C_(2)H_(2).Dynamic breakthrough ex-periments verify the excellent performance of material in practical CO_(2)/C_(2)H_(2)separation,for CO_(2)/C_(2)H_(2)(50/50 and 1/99,V/V)mixtures can be separated in one step,thus directly generating high purity C_(2)H_(2)(>99.95%),which provides a promising thought for the zeolite-based separation of CO_(2)and C_(2)H_(2).

关键词： Zeolite Carbon dioxide Gas separation Electrostatic potential Kinetic diffusion

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