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Frontiers of chemical Science and Engineering 2024年第3期18卷 63-73页

作者： Mengqing Shan Dongsheng Lu Jiatong Dong Shen Yan Jinyu Han Hua Wang Collaborative Innovation Center of chemical Science and Engineering Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300354China

Surface engineering and Cu valence regulation are essential factors in improving the C_(2)selectivity during the electrochemical reduction of CO_(2).Herein,we present a sea urchin-like CuO/Cu_(2)O catalyst derived from rhombic dodecahedra Cu_(2)O through one-step oxidation/etching method where the mixed Cu^(+)/Cu^(0)states are formed via in situ reduction during *** combined effects of the morphology and the mixed Cu^(+)/Cu^(0)states on C–C coupling are evaluated by the Faradaic efficiency of C_(2)and the C_(2)/C1 ratio obtained in an H-cell.R-Cu^(O)/Cu_(2)O exhibited 49.5%Faradaic efficiency of C_(2)with a C_(2)/C1 ratio of 3.1 at−1.4 V *** hydrogen electrode,which are 1.5 and 3.2 times higher than those of R-Cu_(2)O,*** a flow-cell,68.0%Faradaic efficiency of C_(2)is achieved at a current density of 500 mA·cm^(−2).The formation of the mixed Cu^(+)/Cu^(0)states was confirmed by in situ Raman ***,the sea urchin-like structure provides more active sites and enables faster electron *** a result,the excellent C_(2)production on R-CuO/Cu_(2)O is primarily attributed to the synergistic effects of the sea urchin-like structure and the stable mixed Cu^(+)/Cu^(0)***,this work presents an integrated strategy for developing Cu-based electrocatalysts for C_(2)production through electrochemical CO_(2)reduction.

关键词： CO_(2)electrolysis sea urchin-like structure Cu^(+)/Cu^(0) C_(2)products

Monomeric and self-assembled crystal phases of TNBT

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Rare Metals 2024年第10期43卷 5442-5448页

作者： Yun-Hui Wu Hua-Bei You Wei-Kai Cui Zhi-Qian Cao Xiao Dong Zi-Hui Meng Ming Huang school of Chemistry and chemical Engineering Beijing Institute of Technology Institute of chemical Materials China Academy of Engineering Physics

（3,3′,5,5′-Tetranitro-4,4′-bi-1,2,4-Triazole） TNBT was designed and predicted more than three decades ago as a high energy *** with many other designed molecules,TNBT has not been successfully synthesized and has not been computationally studied in *** this work,theoretical calculations at density functional theory （DFT）level of theory were carried out for both the gas phase molecule and its possible bulk crystal *** （DFT） computations show that TNBT is comparable to CL-20 with high bulk density,

关键词： Density functional theory

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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Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan State Key Laboratory of Materials-Oriented chemical Engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

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

Non-isothermal kinetics and characteristics of calcium carbide nitridation reaction with calcium-based additives

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Frontiers of chemical Science and Engineering 2024年第4期18卷 49-61页

作者： Zhihan Zhang Mengxiao Yu Xiaoyu Zhang Jinli Zhang You Han school of chemical Engineering and Technology Tianjin UniversityTianjin 300350China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China

The nitridation reaction of calcium carbide and N_(2) at high temperatures is the key step in the production of ***,the challenges faced by this process,such as high energy consumption and poor product quality,are mainly attributed to the lack of profound understanding of the *** study aimed to improve this process by investigating the non-isothermal kinetics and reaction characteristics of calcium carbide nitridation reaction at different heating rates(10,15,20,and 30℃·min^(-1))using thermogravimetric *** kinetic equation for the nitridation reaction of additive-free calcium carbide sample was obtained by combining model-free methods and model-fitting *** effect of different calcium-based additives(CaCl_(2) and CaF_(2))on the reaction was also *** results showed that the calcium-based additives significantly reduced reaction temperature and activation energy E_(a) by about 40% with CaF_(2) and by 55%-60% with CaCl_(2).The reaction model f(α)was also changed from contracting volume(R3)to 3-D diffusion models with D3 for CaCl_(2) and D4 for CaF_(2).This study provides valuable information on the mechanism and kinetics of calcium carbide nitridation reaction and new insights into the improvement of the lime-nitrogen process using calcium-based additives.

关键词： lime-nitrogen calcium carbide calciumbased additive thermogravimetric analysis nonisothermal kinetics

Nitrogen-doped carbon dots as photocatalysts for organic synthesis:Effect of nitrogen content on catalytic activity

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Nano Research 2024年第6期17卷 4825-4833页

作者： Kai-Kai Niu Chao-Qun Ma Rui-Zhi Dong Hui Liu Sheng-Sheng Yu Ling-Bao Xing school of Chemistry and chemical Engineering Shandong University of TechnologyZibo 255000China

Regulating the doping of carbon dots(CDs)and the generation of reactive oxygen species(ROS)is essential to selectively control their application in photocatalytic organic *** study successfully synthesized five newly developed nitrogen-doped carbon dots(CDs 1-5)with varying nitrogen content,which have the ability to generate ROS when exposed to light radiation,specifically superoxide anion radicals(O_(2)•-)and singlet oxygen(^(1)O_(2)).The utilization of the aforementioned nitrogen-doped CDs as photocatalysts enables the realization of their potential in facilitating efficient photocatalytic organic ***,it was observed that the photocatalytic efficiency exhibited a gradual decrease when the nitrogen content in the CDs *** order to provide more evidence for this claim,we employed a set of five CDs in the context of photocatalytic dehalogenation ofα-bromoacetophenone,photocatalytic oxidative coupling reaction of amines to imines,photooxidation reaction of sulfides to sulfoxides,and cross-dehydrogenation coupling(CDC)reaction,in which it was further observed that there was a steady decrease in the yields of photocatalytic organic reactions as the nitrogen content in CDs ***,CDs 1 exhibited the best photocatalytic efficiency,thereby reinforcing the hypothesis that a higher nitrogen content corresponds to a decreased catalytic *** study not only investigates the impact of the nitrogen content on the catalytic performance of CDs,but also offers valuable insights for the future utilization of CDs for photocatalytic organic reactions in water.

关键词： carbon dots nitrogen-doped reactive oxygen species photocatalysis

Metal–phenolic coordination crystals derived magnetic hollow carbon spheres for ultrahigh electromagnetic wave absorption

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Nano Research 2024年第3期17卷 1616-1624页

作者： Hanxiao Xu Zizhuang He Yiruo Wang Xiangru Ren Panbo Liu school of Chemistry and chemical Engineering Northwestern Polytechnical UniversityXi’an 710129China

Owing to the tunable compositions and versatile functionality,the development of eco-friendly metal–phenolic coordination crystals derivatives is highly anticipated for electromagnetic wave *** this study,three kinds of magnetic hollow carbon spheres(HCSs)with macro-meso-microporous characteristics,including Fe/HCS,Co/HCS,and CoNi/HCS,are successfully fabricated via the co-operative hard template and self-assembling process,in which magnetic particles are encapsulated in carbon shell matrix after the pyrolysis of metal–polyphenol coordination crystals and further subsequent template *** the one hand,hierarchical macro-meso-micropores effectively balance the impedance gap between absorbers and air and introduce structural defects or distortion,leading to matched impedance and enhanced dipolar/defect *** the other hand,wrapped magnetic particles provide uncountable hetero-interfaces and induce ferromagnetic resonance,resulting in strengthened interfacial polarization and additional magnetic *** particular,enhanced minimum reflection loss(RL,min)and broadband effective absorption bandwidth(EAB)are achieved with only 10 wt.%filler ***,the RL,min and EAB values are-57.5 dB and 7.2 GHz for Fe/HCS,-50.0 dB and 5.8 GHz for Co/HCS,and-52.1 dB and 6.7 GHz for CoNi/HCS,***,this work provides us a modular-assembly strategy to regulate the hollow cavity of absorbers and simultaneously manipulates the chemical components of absorbers to regulate electromagnetic wave absorption performance.

关键词： hollow engineering hierarchical pores hetero-interfaces synergetic effect electromagnetic wave absorption

Preparation of a zeolite-palladium composite membrane for hydrogen separation:Influence of zeolite film on membrane stability

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Chinese Journal of chemical Engineering 2024年第8期72卷 44-52页

作者： Hongmei Wu Xinyu Liu Yu Guo school of chemical and Environmental Engineering Liaoning University of TechnologyJinzhou 121001China

With the development of hydrogen energy,palladium-based membranes have been widely used in hydrogen separation and ***,the poor chemical stability of palladium composite membranes limits their commercial *** this study,a zeolite-palladium composite membrane with a sandwich-like structure was obtained by using a TS-1 zeolite film grown on the surface of palladium *** membrane microstructure was characterized by SEM and *** effects of the TS-1 film on the hydrogen permeability and stability of palladium composite membrane were investigated in *** from the protection of the TS-1 zeolite film,the stability of palladium composite membrane was *** results indicate that the TS-1-Pd composite membrane was stable after eight cycles of the temperature exchange cycles between 773 K and 623 ***,the loss of hydrogen permeance for TS-1-Pd composite membrane was much smaller than that of the pure palladium membrane when the membrane was tested in the presence of *** indicated that the TS-1-Pd composite membrane had better chemical stability in comparison with pure palladium membrane,owing to its sandwich-like *** work provides an efficient way for the deposition of zeolite film on palladium membrane to enhance the membrane stability.

关键词： Palladium membrane Zeolite film Hydrogen separation Stability

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Structural Evolution of Ultra-High Molecular Weight Polyethylene Low-Entangled Films with Reserved Shish Crystals During Hot Stretching

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Chinese Journal of Polymer Science 2024年第8期42卷 1227-1242页

作者： Jia-Wei Gao Li Chen Ye-Shun Zhong Chao-Wei Xing Yi-Guo Li Zong-Bao Wang school of Materials Science and chemical Engineering Ningbo UniversityNingbo 315211China

Shish crystals are crucial to achieving high performance low-dimensional ultra-high molecular weight polyethylene(UHMWPE)***,high stretch and shear flow fields are necessary for the formation of shish *** this study,UHMWPE gel films with reserved shish crystals were prepared by gel molding,the structural evolution and properties of UHMWPE films stretched at temperatu res of 100,110,120and 130℃were investigated by in situ small-angle X-ray scattering(SAXS)/ultra-small-angle X-ray scattering(USAXS)/wide-angle X-ray diffraction(WAXD)measu rements as well as scanning electron microscopy(SEM)and differential scanning calorimetry(DSC)*** findings showed that the reserved shish crystals can facilitate the formation and structural evolution of shish-kebab crystals during the hot ***,the reserved shish crystals promote the structu ral evolution of UHMWPE films to a greater extent when stretched at 120 and 130℃,compared to 100 and 110℃,resulting in higher crystallinity,orientation,thermal properties,breaking strength and Young's *** pared to UHMWPE high-entangled films with reserved shish crystals prepared by compression molding,UHMWPE low-entangled films with reserved shish crystals prepared by gel molding are more effective in inducing the formation and evolution of shish-kebab crystals during the hot stretching,resulting in increased breaking strength and Young's modulus.

关键词： UHMWPE low-entangled films Reserved shish crystals Structural evolution Hot stretching

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