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Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu state key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China state key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China state key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

Kinetics and mechanism of propylene hydro-oxidation to acrolein on Au catalysts

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Nano Research 2024年第1期17卷 354-363页

作者： Wei Du Zhihua Zhang Nan Song Xuezhi Duan Xinggui Zhou state key laboratory of chemical engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great *** the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au ***,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and *** Ti sites are found to be non-essential to acrolein ***,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to *** latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental *** work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).

关键词： kinetics mechanism gold acrolein hydro-oxidation

Trace Pd alloyed with Au to boost Au/uncalcined TS-1 catalyzed propane hydro-oxidation to acetone

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Nano Research 2024年第8期17卷 7182-7193页

作者： Jinwei Sun Zhihua Zhang Erchuan Yang Wei Du Fan Liu Kesheng Xu Yuxia Zhong Xuezhi Duan Xinggui Zhou state key laboratory of chemical engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Selective oxidation of propane to acetone(AC)with H_(2) and O_(2) provides a direct route to convert low-cost propane into valueadded ***,the catalytic activity of conventional Au/Ti-based catalysts is constrained by the high energy barrier for H_(2) ***,uncalcined TS-1 supported Au-Pd bimetallic catalysts were prepared,and the relationship between the active-site structure and corresponding performance in the selective oxidation of propane with H_(2) and O_(2) in the gas phase was systematically *** contrast to the liquid-phase reaction,trace Pd alloyed with Au triggered an increase in both catalytic activity and selectivity,in which Au_(20)-Pd_(1)/TS-1-B catalyst exhibited excellent activity(170 gAC·h^(−1)·kgcat^(−1))and AC selectivity(90.6%),much higher than those of the Au/TS-1-B catalyst(AC formation rate of 100 gAC·h^(−1)·kgcat^(−1)and AC selectivity of 86.3%).It was found that Pd was gradually isolated into monomers with the increase of Au/Pd molar ratio,and the synergy between Pd single atoms and Au improved the catalytic performance via enhancing hydrogen dissociation and modulating the electronic structure of ***,the reaction conditions were optimized based on the kinetics studies and the Au_(20)-Pd_(1)/TS-1-B catalyst exhibited enhanced H_(2) selectivity(45%)and long-term stability(over 130 h).The insights gained here can offer valuable guidance for the design of Au-Pd catalysts applicable to other gas-phase oxidation reactions.

关键词： propane selective oxidation acetone hydrogen dissociation Au-Pd alloy synergy

Surface Polarization Effects on Collapse Transition of Polyelectrolyte Brushes

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Chinese Journal of Polymer Science 2024年第9期42卷 1313-1320,I0006页

作者： Xiao-Fei Xu state key laboratory of chemical engineering and school of chemical engineering East China University of Science and TechnologyShanghai200237China

Polyelectrolyte brushes(PEBs)are commonly used to modify surface that have attracted great research *** dielectric permittivity of the grafted surface is typically significantly different from that of solution,which results in surface polarization(SP)effect with a jump of electric *** is thus important to study how SP alters the PEB’s structure and *** this work,the SP effects on PEB structure was studied using a statistical thermodynamic *** free energy functional to describe SP effect was constructed by using the image-charge ***,the electrostatic potential was solved from a modified Poisson-Boltzmann equation taking the ion solvation effect into *** the absence of SP,the thickness of PEB exhibited a continuous collapse transition when decreasing the solvent *** the presence of SP,the collapse became a jump-like *** energy analysis showed that the long-range Coulombic interaction dominated the transition because of the enhanced counterion condensation in the presence of *** theory provides an effective tool to study SP effect on PEBs,and the results explain the underlying physics in PEB collapse transition.

关键词： Surface polarization Polyelectrolyte brush Image charge Ion solvation Polyelectrolyte collapse transition

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The flow behavior of droplet adsorption on a liquid-liquid interface accompanied by cross-linking reaction and phase separation in a microchannel

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Chinese Journal of chemical engineering 2024年第2期66卷 60-70页

作者： Haozhe Yi Taotao Fu Chunying Zhu Youguang Ma state key laboratory of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical ***,the cross-linking reaction,which is widely used in the field of polymers,can change the physical properties of the fluids and affect the flow behavior accordingly.A configuration of microchannels is designed to conveniently generate uniform droplets in one phase of the parallel *** flow behavior of the adsorption process of sodium alginate droplets on the liquid-liquid interface is investigated,and the subsequent process of phase separation is *** the process of droplet adsorption,the crosslinking reaction occurs synchronously,which makes the droplet viscosity and the elasticity modules of the droplet surface increase,thus affecting the dynamics of the adsorption process and the equilibrium shape of the *** variation of the adsorption length with time is divided into three stages,which all conform to power law *** exponents of the second and third stages deviate from the results of the Tanner's *** flow pattern maps of droplet adsorption and phase separation are drawn,and the operating ranges of complete adsorption and complete separation are *** study provides a theoretical basis for further studying the flow behavior of droplets with cross-linking reaction in a microchannel.

关键词： Microfluidics Droplet Dynamics Crosslink Adsorption Separation

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu state key laboratory Base of Eco-chemical engineering College of chemical engineering Qingdao University of Science and TechnologyQingdao266042China key laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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Tailoring NH4+ storage by regulating oxygen defect in ammonium vanadate

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Green Energy & Environment 2024年第7期9卷 1171-1182页

作者： Yanyan Liu Ziyi Feng Hanmei Jiang Xueying Dong Changgong Meng Yifu Zhang state key laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology College of Environmental and chemical engineering Dalian University

Defect engineering is an effective strategy for modifying the energy storage materials to improve their electrochemical ***, the impact of oxygen defect and its content on the electrochemical performances in the burgeoning aqueous NH+4storage field remains explored. Therefore, for the first time in this work, an oxygen-defective ammonium vanadate [（NH4）2V10O25·8H2O, denoted as Od-NHVO] with a novel 3D porous flower-like architecture was achieved via the reduction of thiourea in a mild reaction condition, which is a facile method that can realize the intention to regulate the oxygen defect content, with the capability of mass-production. The as-prepared OdM-NHVO with moderate oxygen defect content can deliver a stable specific capacitance output(505 F g-1, 252 mAh g-1at 0.5 A g-1with ～80% capacitance retention after 10,000 cycles), which benefits from extra active sites, unimpeded NH+4-migration path and relatively high structure integrity. In contrast, low oxygen defect content will lead to the torpid electrochemical reaction kinetics while too high content of it will reduce the chargestorage capability and induce structural disintegration. The superior NH+4-storage behavior is achieved with the reversible intercalation/deintercalation process of NH+4accompanied by forming/breaking of hydrogen bond. As expected, the assembled flexible OdM-NHVO//PTCDI quasi-solid-state hybrid supercapacitor（FQSS HSC） also exhibits high areal capacitance, energy density and reliable flexibility. This work provides a new avenue for developing materials with oxygen-deficient structure for application in various aqueous non-metal cation storage systems.

关键词： Ammonium vanadate Oxygen defect Ammonium-ion storage Hybrid supercapacitors Electrochemical performance

Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The state key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

Optimization of biofuel supply chain integrated with petroleum refineries under carbon trade policy

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Frontiers of chemical Science and engineering 2024年第3期18卷 113-122页

作者： Wenhui Zhang Yiqing Luo Xigang Yuan chemical engineering Research Center School of Chemical Engineering and TechnologyTianjin UniversityTianjin300350China state key laboratory of chemical engineering Tianjin UniversityTianjin300350China

The use of fossil fuels results in significant carbon dioxide *** have been increasingly adopted as sustainable alternatives to fossil fuel to address this environmental *** petroleum refineries into biofuel supply chains is an effective approach to mitigating greenhouse gas emissions and improving environmental *** this study,an integrated supply chain optimization framework was established,considering the carbon trade *** addition,a mixed-integer nonlinear programming model was developed to optimize the selection of biomass suppliers,construction of pretreatment plants and biorefineries,integration of petroleum refineries,and selection of transportation routes with the objective of minimizing the total annual *** example is presented to illustrate the applicability of the *** optimization results show that integrating petroleum refineries into biofuel supply chains effectively mitigates carbon *** trade policies can have a direct impact on the total annual cost and carbon emissions of the supply chain.

关键词： renewable energy biofuel supply chain carbon trade policy