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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

Development of High-Energy-Density Liquid Aerospace Fuel:A Perspective

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Transactions of Tianjin University 2022年第1期28卷 1-5页

作者： Jiaorong Nie Tinghao Jia 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

Aerospace aircraft has significantly improved the life quality of human beings and extended the capability of space explosion since its appearance in 1903,in which liquid propellants or fuels provide the key power *** jet fuels,its property of energy density plays an important role in determining the flight range,load,and performance of the ***,the design and fabrication of high-energy-density(HED)fuels attract more and more attention from researchers all over the ***,we briefly introduce the development of liquid jet fuels and HED fuels and demonstrate the future development of HED *** further improve the energy density of fuel,the approaches of design and construction of multi-cyclic and stained molecule structures are *** break through the density limit of hydrocarbon fuels,the addition of energetic nanoparticles in HED fuels to produce nanofluid or gelled fuels may provide a facile and effective method to significantly increase the energy *** work provides the perspective for the development of HED fuels for advanced aircrafts.

关键词： Liquid aerospace fuel High-energy-density fuel Stained molecule structure Nanofluid or gelled fuels

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

Coupling ferromagnetic ordering electron transfer channels and surface reconstructed active species for spintronic electrocatalysis of water oxidation

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Journal of Energy Chemistry 2023年第10期85卷 570-580,I0014页

作者： Zexing He Xiaokang Liu Minghui Zhang Lei Guo Muhammad Ajmal lun pan Chengxiang Shi Xiangwen Zhang Zhen-Feng Huang 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 Ningbo 315201ZhejiangChina Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_(2-x)Ni_xO_(4)(0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic(FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni^(3+)increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_(1.6)Ni_(0.4)O_(4) shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe_(2)O_(4) and unactivated ZnFe_(1.6)Ni_(0.4)O_(4), and even superior to the benchmark IrO_(2) under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe_(2)O_(4). We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.

关键词： Oxygen evolution reaction Reconstruction mechanism Metal oxyhydroxides Electron transfer channels Ferromagnetic exchange-field penetration

Regulating the interfacial charge transfer and constructing symmetry-breaking sites for the enhanced N_(2) electroreduction activity

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Carbon Energy 2023年第2期5卷 193-200页

作者： Xiaoxue Zhang Yuehan Cao Zhen-Feng Huang Shishi Zhang Chengguang Liu lun pan Chengxiang Shi Xiangwen Zhang Ying Zhou Guidong Yang Ji-Jun Zou Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjinChina Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) TianjinChina Zhejiang Institute of Tianjin University NingboZhejiangChina State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation School of New Energy and MaterialsInstitute of Carbon NeutralitySouthwest Petroleum UniversityChengduSichuanChina XJTU-Oxford International Joint Laboratory for Catalysis School of Chemical Engineering and TechnologyXi'an Jiaotong UniversityXi'anShaanxiChina

The Haber-Bosch process for industrial NH_(3) production is energy-intensive with heavy CO_(2) *** N_(2) reduction reaction(NRR)is an attractive carbon-neutral alternative for NH_(3) synthesis,while the challenge associated with N_(2) activation highlights the demand for efficient ***,we demonstrate that PdCu nanoparticles with different Pd/Cu ratios anchored on boron nanosheet(PdCu/B)behave as efficient NRR electrocatalysts toward NH_(3) *** and experimental results confirm that the highly efficient NH_(3) synthesis can be achieved by regulating the charge transfer between interfaces and forming a symmetry-breaking site,which not only alleviates the hydrogen evolution but also changes the adsorption configuration of N_(2) and thus optimizes the reaction pathway of NRR over the separated Pd *** with monometallic Pd/B and Cu/B,the PdCu/B with the optimized Pd/Cu ratio of 1 exhibits superior activity and selectivity for NH_(3) *** study provides new insight into developing efficient catalysts for small energy molecule catalytic conversion via regulating the charge transfer between interfaces and constructing symmetry-breaking sites.

关键词： catalyst design electrochemical N_(2)reduction interfacial charge transfer reaction mechanism symmetry-breaking sites

Recent Advances in the Comprehension and Regulation of Lattice Oxygen Oxidation Mechanism in Oxygen Evolution Reaction

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天津大学学报:英文版 2023年第4期29卷 247-253页

作者： Xiaokang Liu Zexing He Muhammad Ajmal Chengxiang Shi Ruijie Gao lun pan Zhen‑Feng Huang Xiangwen Zhang Ji‑Jun Zou Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyInstitute of Molecular PlusTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Zhejiang Institute of Tianjin University Ningbo 315201ZhejiangChina

Water electrolysis,a process for producing green hydrogen from renewable energy,plays a crucial role in the transition toward a sustainable energy landscape and the realization of the hydrogen *** evolution reaction(OER)is a critical step in water electrolysis and is often limited by its slow *** main mechanisms,namely the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM),are commonly considered in the context of ***,designing efficient catalysts based on either the AEM or the LOM remains a topic of debate,and there is no consensus on whether activity and stability are directly related to a certain *** the above,we discuss the characteristics,advantages,and disadvantages of AEM and ***,we provide insights on leveraging the LOM to develop highly active and stable OER catalysts in *** instance,it is essential to accurately differentiate between reversible and irreversible lattice oxygen redox reactions to elucidate the ***,we discuss strategies for effectively activating lattice oxygen to achieve controllable steady-state exchange between lattice oxygen and an electrolyte(OH^(-)or H_(2)O).Additionally,we discuss the use of in situ characterization techniques and theoretical calculations as promising avenues for further elucidating the LOM.

关键词： Water electrolysis Oxygen evolution reaction(OER) Adsorbate evolution mechanism(AEM) Lattice oxygen oxidation mechanism(LOM)

Removal of VOCs from gas streams with double perovskite-type catalysts

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Journal of Environmental Sciences 2018年第7期30卷 205-216页

作者： Kuan lun pan Guan Ting pan Siewhui Chong Moo Been Chang Graduate Institute of Environmental Engineering National Central University Department of Chemical Engineering National Taipei University of Technology Department of Chemical and Environmental Engineering University of Nottingham Malaysia Campus

Double perovskite-type catalysts including La2 CoMnO6 and La2 CuMnO6 are first evaluated for the effectiveness in removing volatile organic compounds（VOCs）, and single perovskites（La CoO3, LaMnO3, and La Cu O3） are also tested for comparison. All perovskites are tested with the gas hourly space velocity（GHSV） of 30,000 hr^-1, and the temperature range of100–600℃ for C7H8 removal. Experimental results indicate that double perovskites have better activity if compared with single perovskites. Especially, toluene（C7H8） can be completely oxidized to CO2 at 300℃ as La2 Co MnO6 is applied. Characterization of catalysts indicates that double perovskites own unique surface properties and are of higher amounts of lattice oxygen,leading to higher activity. Additionally, apparent activation energy of 68 k J/mol is calculated using Mars-van Krevelen model for C7 H8 oxidation with La2 Co Mn O6 as catalyst. For durability test, both La2 Co Mn O6 and La2 CuMnO6 maintain high C7 H8 removal efficiencies of 100% and98%, respectively, at 300℃ and 30,000 hr^-1, and they also show good resistance to CO2（5%） and H2 O（g）（5%） of the gas streams tested. For various VOCs including isopropyl alcohol（C3H8 O）,ethanal（C2H4O）, and ethylene（C2H4） tested, as high as 100% efficiency could be achieved with double perovskite-type catalysts operated at 300–350℃, indicating that double perovskites are promising catalysts for VOCs removal.

关键词： Volatile organic compounds(VOCs) Toluene(C7H8) Double perovskite-type catalyst Catalysis Activation energy