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Structural Engineering of Anode materials for Low-Temperature Lithium-Ion Batteries:Mechanisms,Strategies,and Prospects

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Nano-Micro Letters 2024年第8期16卷 169-195页

作者： Guan Wang Guixin Wang Linfeng Fei Lina Zhao Haitao Zhang beijing key laboratory of Ionic Liquids Clean process Institute of Process EngineeringChinese Academy of SciencesBeijing 100190People’s Republic of China School of Chemical Engineering Sichuan UniversityChengdu 610065People’s Republic of China School of Energy materials and Chemical Engineering Hefei UniversityHefei 230601People’s Republic of China School of materials Science and Engineering Nanchang UniversityNanchang 330031People’s Republic of China key laboratory of Polymer and Catalyst Synthesis technology of Liaoning Province School of Environmental and Chemical EngineeringShenyang University of TechnologyShenyang 110870People’s Republic of China

The severe degradation of electrochemical performance for lithium-ion batteries(LIBs)at low temperatures poses a significant challenge to their practical applications.Consequently,extensive efforts have been contributed to explore novel anode materials with high electronic conductivity and rapid Li^(+)diffusion kinetics for achieving favorable low-temperature performance of LIBs.Herein,we try to review the recent reports on the synthesis and characterizations of low-temperature anode materials.First,we summarize the underlying mechanisms responsible for the performance degradation of anode materials at subzero temperatures.Second,detailed discussions concerning the key pathways(boosting electronic conductivity,enhancing Li^(+)diffusion kinetics,and inhibiting lithium dendrite)for improving the low-temperature performance of anode materials are presented.Third,several commonly used low-temperature anode materials are briefly introduced.Fourth,recent progress in the engineering of these low-temperature anode materials is summarized in terms of structural design,morphology control,surface&interface modifications,and multiphase materials.Finally,the challenges that remain to be solved in the field of low-temperature anode materials are discussed.This review was organized to offer valuable insights and guidance for next-generation LIBs with excellent low-temperature electrochemical performance.

关键词： Low-temperature performance Anode materials Microstructural regulations Surface modifications

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Fabrication of CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2) photocatalyst with intrinsic p-n junction for highly efficient bisphenol A degradation

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Journal of Environmental Sciences 2024年第2期136卷 547-558页

作者： Yong Wang Cheng Liu Haoyun Hu Qiujun Lu Haiyan Wang Chenxi Zhao Fuyou Du Ningli Tang Guangxi key laboratory of electrochemical and Magnetochemical Functional materials College of Chemistry and BioengineeringGuilin University of TechnologyGuilin 541004China College of Biological and Environmental Engineering Changsha UniversityChangsha 410022China

The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant removal.In this work,a novel CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)photocatalysts were synthesized by simple hydrothermal and chemical precipitation method.The fabricated CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)composite exhibited much higher photocatalytic activity than pristine CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2)in the removal of bisphenol A(BPA)under visible-light illumination,which ascribed to the intrinsic p-n junction of CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2).The photocatalytic degradation rate of BPA on CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)with an optimized CuFe_(2)O_(4)content(1.0 wt.%)reached 93.0%within 30 min.The capture experiments of active species confirmed that the hydroxyl radicals(·OH)and superoxide radicals(·O_(2)^(-))played crucial roles in photocatalytic BPA degradation process.Furthermore,the possible degradation mechanism and pathways of BPA was proposed according to the detected intermediates in photocatalytic reaction process.

关键词： Bi_(12)O_(17)Cl_(2) CuFe_(2)O_(4) Heterojunction Bisphenol A Photocatalytic degradation

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Silicon dioxide-protection boosting the peroxidase-like activity of Fe single-atom catalyst for combining chemo-photothermal therapy

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Nano Research 2024年第6期17卷 4924-4933页

作者： Yu Fan Yu Yi Hongpan Rong Jiatao Zhang beijing key laboratory of Construction-Tailorable Advanced Functional materials and Green Applications School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China CAS Center for Excellence in Nanoscience CAS KeyLaboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing 100190China key laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologySchool of Chemistry&Chemical EngineeringBeijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green ApplicationsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Carbon-based single-atom catalysts(SACs)have been widely studied in the field of biomedicine due to their excellent catalytic performance.However,carbon-based SACs usually aggregate during pyrolysis,which leads to the reduction of catalytic activity.Here,we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer.The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles,which is not destroyed during the pyrolysis process,ensuring the single-particle dispersion of the nanoparticles after etching.This approach increased the hydroxyl groups on the surface of Fe-SAC(Fe-SAC-SE)and improved its water solubility,resulting in a four times enhancement of the peroxidase(POD)-like activity of Fe-SAC-SE(58.4 U/mg)than that of non-protected SACs(13.9 U/mg).The SiO_(2)-protection approach could also improve the catalytic activities of SACs with other metals such as Mn,Co,Ni,and Cu,indicating its generality for SACs preparation.Taking advantage of the high POD-like activity,photothermal properties,and large specific surface area of Fe-SAC-SE,we constructed a synergistic therapeutic system(Fe-SAC-SE@DOX@PEG)for combining the photothermal therapy,catalytic therapy,and chemotherapy.It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity,exhibiting excellent tumor-killing performance at the cellular level.This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.

关键词： single-atom catalysts peroxidase-like activity SiO2-protection photothermal therapy catalytic therapy chemotherapy

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A flame-retardant binder with high polysulfide affinity for safe and stable lithium–sulfur batteries

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Science China Chemistry 2024年第3期67卷 1028-1036页

作者： Guowei Yu Guofeng Ye Cheng Wang Chenyang Wang Zhaoyun Wang Pu Hu Yu Li Xi-Xi Feng Shuang-Jie Tan Min Yan Sen Xin Zhitian Liu Hubei key laboratory of Plasma Chemistry and Advanced materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China State key laboratory of Advanced technology for materials Synthesis and processing Wuhan University of TechnologyWuhan 430070China CAS key laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.

关键词： lithium–sulfur battery polymer binder polysulfide affinity flame retardancy

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Optimal V_(2)O_(3) extraction by sustainable vanadate electrolysis in molten salts

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Tungsten 2024年第1期6卷 141-149页

作者： Bao-Yan Feng Zhong-Hua Zhao Yong-Zheng Jia Jia-Liang An Ming-Yong Wang State key laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China beijing key laboratory of Green Recovery and Extraction of Rare and Precious Metals University of Science and Technology BeijingBeijing 100083China

Recently,an environmentally friendly electrolysis process of soluble vanadates is proposed and successfully confirmed for V_(2)O_(3) extraction.In this paper,the solubilities of various vanadates(i.e.NaVO_(3),Na_(4)V_(2)O_(7) and Na_(3)VO_(4))in NaCl molten salt are measured.The dependences of V_(2)O_(3) extraction on vanadate form,anode material and molten salt system are studied.A long-term electrolysis is carried out.The result indicates that the solubilities of all vanadates are high and meet electrolytic requirements.Compared to Na_(4)V_(2)O_(7) and Na_(3)VO_(4),NaVO_(3) exhibits larger current efficiency and lower electricity consumption.By using SnO_(2) anode instead of graphite anode,the current efficiency of NaVO_(3) electrolysis can be increased to 58.1%and carbon pollution is avoided at 700℃.The extraction rate of V_(2)O_(3) reaches 81.3%after long-term electrolysis of 51 h.This work optimizes the electrochemical preparation process of V_(2)O_(3) from various vanadates and contributes to the improvement of current efficiency and extraction rate.

关键词： Molten salt electrolysis Vanadate Vanadium trioxide Current efficiency

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Mechanical reliable,NIR light-induced rapid self-healing hydrogel electrolyte towards flexible zinc-ion hybrid supercapacitors with low-temperature adaptability and long service life

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Journal of Energy Chemistry 2024年第5期92卷 63-73页

作者： Tengjia Gao Na Li Yang Yang Jing Li Peng Ji Yunlong Zhou Jianxiong Xu School of materials and Advanced Manufacturing Hunan Key Laboratory of Electrochemical Green Metallurgy TechnologyHunan University of TechnologyZhuzhou 412007HunanChina School of Life Sciences and Chemistry Hunan Key Laboratory of Biomedical Nanomaterials and DevicesHunan University of TechnologyZhuzhou 412007HunanChina

Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.

关键词： Flexible zinc ion supercapacitor Hydrogel electrolyte Self-healing Anti-freezing

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Application of surfactant for improving leaching process of weathered crust elution-deposited rare earth ores

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Journal of Rare Earths 2024年第1期42卷 181-190,I0007页

作者： Fang Zhou Lisen Zhang Zhiwei Wang Yixin Zhang Ru'an Chi Xiaoyan Wu key laboratory for Green Chemical process of Ministry of Education Wuhan Institute of TechnologyWuhan430073China

Weathered crust elution-deposited rare earth ores(WREOs)in China are the main source of medium and heavy rare earths in the world.In order to improve the seepage and the mass transfer of traditional ammonium salt leaching process of WREOs,surfactants were added in the ammonium sulfate leaching solution and the ammonium chloride leaching solution.The leaching kinetics,the mass transfer process,and the adhesion work reduction factor calculated from the interfacial properties were studied to reveal the strengthening mechanism of surfactant.In the presence of the tested five surfactants,cetyl trimethyl ammonium bromide(CTAB),dodecyl trimethyl ammonium bromide(DTAB),sodium dodecyl sulfate(SDS),sodium oleate and oleic acid,the permeability of WREOs is improved,the rare earth(RE)leaching efficiency increase and the impurity aluminum(Al)leaching efficiency decrease,indicating its promotional effect on the leaching process of WREOs.Furthermore,CTAB shows a better leaching enhancement,and the optimal addition dosage is 0.4 g/L for the two ammonium salt leaching agent systems.The kinetics analysis shows the internal diffusion controls model of RE and Al leaching process,and the leaching kinetics equations of RE and Al related to CTAB concentration were obtained for the two ammonium salt leaching systems.According to the chromatographic plate theory,the mass transfer efficiency of RE increases with the CTAB concentration increasing until 0.4 g/L,which confirms that the optimal CTAB addition is 0.4 g/L.Smaller adhesion work and adhesion work reduction factor indicate more favorable permeation as well as the leaching process.

关键词： Weathered crust elution-deposited rare earth ores Surfactant Kinetics Mass transfer

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Electron-distribution control via Pt/NC and MoC/NC dual junction:Boosted hydrogen electro-oxidation and theoretical study

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Journal of Energy Chemistry 2024年第1期88卷 513-520,I0011页

作者： Feng Zhou Xiaofeng Ke Yihuang Chen Mei Zhao Yun Yang Youqing Dong Chao Zou Xi’an Chen Huile Jin Lijie Zhang Shun Wang key laboratory of Carbon materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325000ZhejiangChina Zhejiang Engineering Research Center for electrochemical Energy materials and Devices Institute of New Materials&Industry TechnologyWenzhou UniversityWenzhou 325000ZhejiangChina

The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO.

关键词： Hydrogen oxidation reaction Dual junctions CO-tolerance Platinum

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Catalytic Reaction Kinetics of Propylene Dimerization to 4-Methyl-1-Pentene Using Cu-K/K_(2)CO_(3) Solid Base Catalyst

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China Petroleum processing & Petrochemical technology 2024年第1期26卷 78-87页

作者： Jin Haibo Chai Jing Yang Suohe He Guangxiang Ma Lei Guo Xiaoyan College of New materials and Chemical Engineering Beijing Institute of Petrochemical Technology/Beijing Key Laboratory of Fuel Cleaning and Efficient Catalytic Emission Reduction TechnologyBeijing102617China

The catalysis technology of propylene dimerization to form 4-methyl-1-pentene(4MP1)using a Cu-K/K_(2)CO_(3) solid base catalyst is a well-known heterogeneous catalytic reaction.In this study,the intrinsic kinetics of propylene dimerization were studied in a fixed-bed continuous reactor.Internal and external diffusion during the dimerization reaction experiments were eliminated by adjusting the flow rate of the carrier gas and the particle size of the catalyst support.Then,the concentration changes of each substance at the outlet of the catalyst bed under different residence times were investigated.Moreover,the suitable reaction kinetics equations was derived using the Langmuir Hinshelwood-Hougen-Watson kinetic model.Finally,the activation energy for each reaction involved in the dimerization reaction was calculated.The activation energies of 4MP1,branched by-products,and 1-hexene were 115.0,150.8,and 177.4 kJ/mol,respectively.The effect of process conditions on propylene dimerization with solid base catalysts was studied through kinetic model simulation.By comparing the theoretical values obtained from the simulation with the experimental results,the applicability and accuracy of the kinetic model were verified.

关键词： propylene dimerization 4-methyl-1-pentene intrinsic kinetics surface reaction

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Alternative technology for the recovery of butyl acetate with low concentration:high capacity adsorbent and high efficiency adsorption

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Green Chemical Engineering 2024年第2期5卷 236-244页

作者： Chi Ma Lihong Zhao Zhengxin Mao Hao Su Qingfen Liu CAS key laboratory of Green process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Industrial pharmaceutical wastewater usually contains butyl acetate(BA)with a concentration of 1 wt%-7 wt%,and the traditional method for BA recovery is distillation with high energy consumption.Adsorption method is developed to recover BA with low concentration for the high efficiency and low energy consumption.Medium polar polyacrylate resins with macroporous structure of 233.1 nm and average particle size of about 526.5μm are successfully synthesized by suspension polymerization and used for the BA adsorption and desorption.The maximum adsorption capacity reaches 171.1 mg g^(-1)with relative standard deviation(RSD)value of 0.2%,which is more than twice the results in the literature.The BA desorption rate is 97.0%at 100℃with RSD value of 0.4%,and the resins are beneficial to the reuse in the adsorption-desorption cycle.The adsorption thermodynamics and kinetics are investigated,and the BA adsorption is a spontaneous and endothermic process with the increase of disorder degree.This process is mainly contributed by physical absorption and agree well with Freundlich model and pseudo-first-order adsorption kinetic model.The adsorption method avoids boiling a large amount of wastewater and hopefully provides a novel alternative technology for the BA recovery.

关键词： Butyl acetate recovery Resin adsorption Desorption Thermodynamics Kinetics

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