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Solid-conversion synthesis of three-dimensionally ordered mesoporous ZSM-5 catalysts for the methanol-to-propylene reaction

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Frontiers of chemical Science and engineering 2024年第8期18卷 111-122页

作者： Weilong Chun Chenbiao Yang Xu Wang Xin Yang Huiyong Chen school of chemical engineering Northwest UniversityXi’an 710069China International Science&Technology Cooperation Base for Clean Utilization of Hydrocarbon Resources Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei EnergyCollaborative Innovation Center for Development of Energy and Chemical Industry in Northern ShaanxiNorthwest UniversityXi’an 710069China

A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity(3DOm ZSM-5)was achieved by solid conversion(SC)of SiO_(2)colloidal crystals to high-crystalline *** products of 3DZ5_S/C and 3DZ5_S,which were severally transformed from the carbon-padded SiO_(2)colloidal crystals and the initial SiO_(2)colloidal crystals,exhibited not only a similar ordered structure and acidity but also higher crystallinity and more balanced meso-/micropore combination in comparison with 3DZ5_C obtained by the conventional confined space crystallization *** three synthesized 3DZ5 catalysts showed improved methanol-to-propylene performance than the commercially microporous ZSM-5(CZ5),embodied in five times longer lifetime,higher propylene selectivity and S_(propylene)/S_(ethylene) ratio(P/E),and superior coke toleration with lower formation rate of coke(R_(coke)).Moreover,the 3DZ5_S catalyst in situ converted from SiO_(2)colloidal crystals presented the highest selectivities of propylene(42.51%)and light olefins(74.6%)among all three 3DZ5 *** high efficiency in synthesis and in situ utilization of SiO_(2)colloidal crystals demonstrate the proposed SC strategy to be more efficiently and eco-friendly for the high-yield production of not only 3DOm ZSM-5 but also other types of hierarchical zeolites.

关键词： hierarchical zeolite three-dimensionally ordered mesoporosity ZSM-5 solid conversion methanol-to-propylene

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chemical looping reforming of the micromolecular component from biomass pyrolysis via Fe_(2)O_(3)@SBA-16

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International Journal of Coal Science & Technology 2024年第3期11卷 120-134页

作者： Yunchang Li Bo Zhang Xiantan Yang Bolun Yang Shengyong Zhang Zhiqiang Wu Shaanxi Key Laboratory of energy chemical Process Intensification School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an710049ShaanxiPeople’s Republic of China

To solve the problems of low gasification efficiency and high tar content caused by solid–solid contact between biomass and oxygen carrier in traditional biomass chemical looping gasification *** decoupling strategy was adopted to decouple the biomass gasification process,and the composite oxygen carrier was prepared by embedding Fe_(2)O_(3) in molecular sieve SBA-16 for the chemical looping reforming process of pyrolysis micromolecular model compound methane,which was expected to realize the directional reforming of pyrolysis volatiles to prepare hydrogen-rich *** analysis of the reaction system was carried out based on the Gibbs free energy minimization method,and the reforming performance was evaluated by a fixed bed reactor,and the kinetic parameters were solved based on the gas–solid reaction *** analysis verified the feasibility of the reaction and provided theoretical guidance for experimental *** experimental results showed that the reaction performance of Fe_(2)O_(3)@SBA-16 was compared with that of pure Fe_(2)O_(3) and Fe_(2)O_(3)@SBA-15,and the syngas yield was increased by 55.3%and 20.7%respectively,and it had good cycle *** analysis showed that the kinetic model changed from three-dimensional diffusion to first-order reaction with the increase of *** activation energy was 192.79 kJ/mol by *** paper provides basic data for the directional preparation of hydrogen-rich syngas from biomass and the design of oxygen carriers for pyrolysis of all-component chemical looping reforming.

关键词： Biomass pyrolysis Methane chemical looping reforming Oxygen carrier Kinetic analysis

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Photocatalytic ozonation-based degradation of phenol by ZnO—TiO_(2)nanocomposites in spinning disk reactor

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Chinese Journal of chemical engineering 2024年第8期72卷 74-84页

作者： Xueqing Ren Jiahao Niu Yan Li Lei Li Chao Zhang Qiang Guo Qiaoling Zhang Weizhou Jiao Shanxi Province Key Laboratory of Higee-Oriented chemical engineering School of Chemistry and Chemical EngineeringNorth University of ChinaTaiyuan 030051China Shanxi Sanqiang New energy Technology Co. LtdTaiyuan 030051China

Spinning disk reactor(SDR)has emerged as a novel process intensification photocatalytic reactor,and it has higher mass transfer efficiency and photon utilization for the degradation of toxic organic pollutants by advanced oxidation processes(AOPs).In this study,ZnO—TiO_(2)nanocomposites were prepared by solgel method,and coated on the disk of SDR by impregnation-pull-drying-calcination *** performance of catalyst was characterized by X-ray diffraction,scanning electron microscope,X-ray photoelectron spectroscopy,photoluminescence and ultraviolet—visible diffuse reflectance *** ozonation in SDR was used to remove phenol,and various factors on degradation effect were studied in *** results showed that the rate of degradation and mineralization reached 100%and 83.4%under UV light irradiation after 50 min,compared with photocatalysis and ozonation,the removal rate increased by 69.3%and 34.7%,and mineralization rate increased by 56.7%and 62.9%,which indicated that the coupling of photocatalysis and ozonation had a synergistic *** radical capture experiments demonstrated that the active species such as photogenerated holes(h^(+)),hydroxyl radicals(·OH),superoxide radical(·O_(2)-)were responsible for phenol degradation,and·OH played a leading role in the degradation process,while h+and·O_(2)^(-)played a non-leading role.

关键词： Spinning disk reactor Photocatalytic ozonation ZnO-TiO_(2)nanocomposites Advanced oxidation processes

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A highly stable zinc anode protected by a corrosion inhibitor for seawater-based zinc-ion batteries

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Journal of energy Chemistry 2024年第10期97卷 332-341页

作者： Bowei Shi Rongwei Meng Xin Jiang Yingxin Liu Huaiyuan Wang Quanjun Tang Li Wang Chen Zhang Guowei Ling Quan-Hong Yang Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage State Key Laboratory of Chemical Engineering School of Chemical Engineering and Technology National Industry-Education Integration Platform of Energy Storage Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)Tianjin University Joint school of National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of Sustainable chemical Transformations school of Marine Science and Technology Tianjin University

The island-based energy storage is of urgent need for the grid construction combined with renewable energy for offshore *** direct use of seawater as a substitute of deionized water shows its great promise for aqueous zinc-ion batteries in such a specific ***,the metal corrosion,dendrite growth,and hydrogen evolution stand out in the harsh seawater *** address these challenges,we proposed a corrosion inhibitor that was effective in the field of metal anti-corrosion,2-phosphonobutane-1,2,4-tricarboxylic acid（PBTCA）,to inhibit anode corrosion caused by Cl-and active H2O molecules by forming a stable solid electrolyte interphase（SEI） film in the seawater-based ***,PBTCA can chelate with other cations present in seawater,such as Ca2+and Mg2+,thereby preventing the aggregation and precipitation of sparingly soluble *** a current density of5 mA cm-2,the seawater-based zinc-ion battery exhibited an exceptional cycle life exceeding 2000 h and maintained a Coulombic efficiency of over 99.6% after 2000 ***,the performance of the Zn||ZVO full battery was significantly enhanced with the addition of *** study provides a simple,low-cost,and efficient approach for making the seawater-based zinc-ion batteries useable.

关键词： Anti-corrosion Seawater Solid electrolyte interphase Zinc-ion batteries

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Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

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National Science Review 2024年第2期11卷 168-176页

作者： Xiaowei Du Peng Zhang Gong Zhang Hui Gao Lili Zhang Mengmeng Zhang Tuo Wang Jinlong Gong school of chemical engineering and Technology Key Laboratory for Green Chemical Technology of the Ministry of Education Tianjin University Collaborative Innovation Center of chemical Science and engineering(Tianjin) National Industry-Education Platform of energy Storage Tianjin University Joint school of the National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of Sustainable chemical Transformations

Gas diffusion electrodes（GDEs） mediate the transport of reactants, products and electrons for the electrocatalytic CO2reduction reaction（CO2RR） in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies（FE > 90%） at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.

关键词： CO2 electroreduction gas diffusion electrode mass transfer ionomer Ag catalyst

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Hard carbon for sodium storage:Mechanism and performance optimization

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Nano Research 2024年第7期17卷 6038-6057页

作者： Yongxin Wang Meng Li Yu Zhang Naiqing Zhang State Key Laboratory of Urban Water Resource and Environment School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China school of energy Science and engineering Harbin Institute of TechnologyHarbin 150001China

Due to the shortage of lithium resource reserves and the pressure of rising prices,sodium-ion batteries have regained the attention of the public,and shown great potential for application in the fields of grid energy storage and low-speed vehicles to achieve the purpose of complementing lithium-ion batteries,so it is imperative to promote the commercial application of sodiumion *** sodium-ion battery anode materials,hard carbon is the material most likely to be used ***,there is still much work to be done before its *** review provides a comprehensive overview of the current research status from the following three ***,the microstructure and sodium storage active sites of hard carbon are ***,the mechanism of sodium storage in hard carbon is investigated,which can be broadly categorized into four model,“insertion–filling”,“adsorption–insertion”,“adsorption–filling”,and“multistage”.Finally,from the perspective of improving the electrochemical performance of hard carbon,the performance improvement strategies proposed in recent years are *** with the performance of hard carbon commercial products of some enterprises,the future development goal of hard carbon is prospected,hoping that all sectors of society can work hard for this common goal.

关键词： sodium-ion battery hard carbon mechanism performance optimization

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Mitigating kinetic hindrance of single-crystal Ni-rich cathodes through morphology modulation, nickel reduction, and lithium vacancy generation achieved by terbium doping

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Journal of energy Chemistry 2024年第10期97卷 566-574页

作者： Jiyuan Jian Shuang Lin Guokang Han Xianglian Zhan Yinghui Shan Rang Xiao Ziwei Liu Dandan Sun Xin Zhang Qingjie Zhou Geping Yin Hua Huo Yulin Ma Pengjian Zuo Xinqun Cheng Chunyu Du State Key Laboratory of Space Power-sources School of Chemistry and Chemical Engineering Harbin Institute of Technology Zibo Torch energy Co.Ltd

Single crystallization has proven to be effective in enhancing the capacity and stability of Ni-rich LiNi1-x-yCoxMnyO2（SNCM） cathode materials,particularly at high cut-off ***,the synthesis of high-quality single-crystal particles remains challenging because of severe particle agglomeration and irregular ***,the limited kinetics of solid-phase Li+diffusion pose a significant concern because of the extended diffusion path in large single-crystal *** address these challenges,we developed a Tb-doped single-crystal LiNi0.83Co0.11Mn0.06O2（SNCM-Tb） cathode material using a straightforward mixed molten salt sintering *** Tb-doped Ni-rich single crystals presented a quasi-spherical morphology,which is markedly different from those reported in previous ***4+oping significantly enhanced the dynamic transport of Li+ions in the layered oxide phase by reducing the Ni valence state and creating Li vacancies.A SNCM-Tb material with 1 at% Tb doping shows a Li+diffusion coefficient up to more than 9 times higher than pristine SNCM in the non-diluted *** situ X-ray diffraction analysis demonstrated a significantly facilitated H1-H2-H3 phase transition in the SNCM-Tb materials,thereby enhancing their rate capacity and structural ***-Tb exhibited a reversible capacity of 186.9 mA h g-1at 5 C,retaining 94.6% capacity after 100 cycles at 0.5 C under a 4,5 V *** study elucidates the Tb4+doping mechanisms and proposes a scalable method for enhancing the performance of single-crystal Ni-rich NCM materials.

关键词： Li+ diffusion kinetics Lithium-ion batteries Ni-rich layered oxides Single crystals Tb4+ doping

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Polymeric hollow fiber membrane for cooling crystallization seeding:On the mechanism of induced nucleation based on thermal transfer Author links open overlay panel

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Particuology 2024年第8期91卷 38-49页

作者： Zeman He Shaofu Du Guanying Shao Peiyu Li Lei Sheng Gaohong He Xiaobin Jiang Wu Xiao State Key Laboratory of Fine chemicals School of Chemical EngineeringEngineering Laboratory for Petrochemical Energy-efficient Separation Technology of Liaoning ProvinceDalian University of TechnologyDalian 116024China

Cooling crystallization is an important separation process and particuology technology that requires accurate nucleation control ***,we introduced the polymeric hollow fiber membrane with proper thermal properties as the effective nucleation induction interface during cooling *** heterogeneous nucleation control mechanism was introduced based on classical nucleation theory and the thermal transfer *** properties and the thermal conductivity of two kinds of polymeric membranes,polytetrafluoroethylene(PTFE)and polyethersulfone(PES),were measured and simulated with the developed *** two membranes possessed different nucleation induction periods,nucleation rates and crystallization performances,which validated that the hollow fiber membrane module could effectively accelerate the nucleation process compared to conventional cooling crystallization owing to the shorter nucleation induction period and the reduced solution surface *** to the higher hydrophobicity and the lower roughness of the membrane surface,the PTFE membrane possessed a more moderate performance in generating stable heterogeneous nucleation than the one of PES ***,the adjustable membrane property enabled the hollow fiber membrane-assisted cooling crystallization to possess the accurate nucleation control and desired terminal particle products.

关键词： Cooling crystallization Nucleation Particle process Hollow fiber membrane Induction period Process control

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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

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Long-term operation optimization of circulating cooling water systems under fouling conditions

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Chinese Journal of chemical engineering 2024年第1期65卷 255-267页

作者： Jiarui Liang Yong Tian Shutong Yang Yong Wang Ruiqi Yin Yufei Wang school of chemical engineering and Environment China University of PetroleumBeijing102249China CHN energy Xinjiang chemical Co. LTDUrumqi830092China College of Mechanical and Transportation engineering China University of PetroleumBeijing 102249China

Fouling caused by excess metal ions in hard water can negatively impact the performance of the circulating cooling water system(CCWS)by depositing ions on the heat exchanger's ***,the operation optimization of CCWS often prioritizes short-term flow velocity optimization for minimizing power consumption,without considering ***,low flow velocity promotes ***,it's crucial to balance fouling and energy/water conservation for optimal CCWS long-term *** study proposes a mixed-integer nonlinear programming(MINLP)model to achieve this *** model considers fouling in the pipeline,dynamic concentration cycle,and variable frequency drive to optimize the synergy between heat transfer,pressure drop,and *** optimizing the concentration cycle of the CCWS,water conservation and fouling control can be *** model can obtain the optimal operating parameters for different operation intervals,including the number of pumps,frequency,and valve local resistance *** experiments on cycle and environmental temperature reveal that as the cycle increases,the marginal benefits of energy/water conservation *** periods with minimal impact on fouling rate,energy/water conservation can be achieved by increasing the cycle while maintaining a low fouling ***,the proposed model has significant energy/water saving effects and can comprehensively optimize the CCWS through its incorporation of fouling and cycle optimization.

关键词： Computer simulation Circulating water system Fouling Concentration cycle Optimization Variable frequency drive

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