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ZnO Additive Boosts Charging Speed and Cycling Stability of Electrolytic Zn–Mn Batteries

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Nano-Micro Letters 2024年第4期16卷 293-304页

作者： Jin Wu Yang Tang Haohang Xu Guandie Ma Jinhong Jiang Changpeng Xian Maowen Xu Shu‑Juan Bao Hao Chen institute for Clean energy&advanced Materials School of Materials and EnergySouthwest UniversityChongqing 400715People’s Republic of China

Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.

关键词： Electrolytic aqueous zinc-manganese batteries Electrolyte pH value ZnO electrolyte additive Fast constant-voltage charging ability

Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors

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Carbon energy 2024年第1期6卷 108-141页

作者： Weiheng Li Qiu-An Huang Yuxuan Bai Jia Wang Linlin Wang Yuyu Liu Yufeng Zhao Xifei Li Jiujun Zhang institute for Sustainable energy/College of Sciences Shanghai UniversityShanghaiChina Shanxi Key Laboratory of Nanomaterials and Nanotechnology School of Mechanical and Electrical EngineeringXi'an University of Architecture and TechnologyXi'anShaanxiChina Xi'an Key Laboratory of New energy Materials and Devices School of Materials Science and EngineeringInstitute of Advanced Electrochemical EnergyXi'an University of TechnologyXi'anShaanxiChina

Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.

关键词： battery,fuel cell,supercapacitor fractional impedance spectroscopy model reduction time-frequency analysis

On-demand engineerable visible spectrum by fine control of electrochemical reactions

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National Science Review 2024年第3期11卷 239-249页

作者： Qirong Liu Lei Liu Yongping Zheng Min Li Baofu Ding Xungang Diao Hui-Ming Cheng Yongbing Tang advanced energy Storage Technology Research Center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences School of energy and Power Engineering North University of China School of Resource Environment and Safety EngineeringHunan University of Science and Technology School of energy and Power Engineering Beihang University Shenzhen Key Laboratory of energy Materials for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences

Tunability of optical performance is one of the key technologies for adaptive optoelectronic applications,such as camouflage clothing, displays, and infrared shielding. High-precision spectral tunability is of great importance for some special applications with on-demand adaptability but remains challenging. Here we demonstrate a galvanostatic control strategy to achieve this goal, relying on the finding of the quantitative correlation between optical properties and electrochemical reactions within materials. An electrochromic electro-optical efficiency index is established to optically fingerprint and precisely identify electrochemical redox reactions in the electrochromic device. Consequently, the charge-transfer process during galvanostatic electrochemical reaction can be quantitatively regulated, permitting precise control over the final optical performance and on-demand adaptability of electrochromic devices as evidenced by an ultralow deviation of electrochemical energy storage, electrocatalysis, and material chemistry.

关键词： electrochromics fine control spectral tunability high precision galvanostatic control

Integration of urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays within porous copper current collector for superior performance Li-ion battery anodes

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Rare Metals 2024年第2期43卷 599-611页

作者： Xue-Ru Zhang Qiong Wu Yong Zhang Xi-Fei Li Ting Xie Yu-Cheng Wu Instrumental Analysis Center Hefei University of TechnologyHefei230009China Key Laboratory of advanced Functional Materials and Devices of Anhui Province Hefei230009China School of Materials Science and Engineering Hefei University of TechnologyHefei230009China institute of advanced electrochemical energy Xi’an University of TechnologyXi’an710048China

Spinel MnCo_(2)O_(4) is a promising energy storage candidate as anode materials in lithium-ion batteries owing to synergistic effects of two intrinsic solid-state redox couples.However,low conductivity,poor rate capacity and rapid capacity fading have seriously impaired its practical applications.To overcome the inferiorities,urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays have been fabricated directly within a porous copper current collector via a facile hydrothermal method followed by a chemical vapor deposition carbonization process.In a typical nanowire,the core is composed of interconnected MnCo_(2)O_(4)nanoparticles and the shell shows as a thin amorphous carbon layer.The integrated MnCo_(2)O_(4)@C/Cu structure could act as working anodes without using additives or polymer binders.While MnCo_(2)O_(4)@C/Cu possesses slightly longer Li-ion insertion/desertion pathway than that of MnCo_(2)O_(4)/Cu,the carbon shell could effectively prevent the pulverization of MnCo_(2)O_(4) and lower down charge transfer resistance and actively participate in Li-ion cycles.The rearrangement of carbon atoms during lithiation/delithiation cycling could inhibit the formation of passive solid electrolyte interphase films.As a result,the MnCo_(2)O_(4)@C/Cu electrode presents superior rate capacity(600 mAh·g^(−1) at 1 A·g^(−1)) and better stability(797 mAh·g^(−1) after 200 cycles at 100 mA·g^(−1)).The excellent reversible Li ion storage capacity,cycling stability and rate capacity endow MnCo_(2)O_(4)@C/Cu great potential as stable and high output integrated anode materials in Li-ion batteries.

关键词： MnCo_(2)O_(4)@C Urchin-like nanowire arrays Core-shell Integrated anode materials Lithium-ion batteries

Characterization and quantification of multi-field coupling in lithium-ion batteries under mechanical constraints

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Journal of energy Chemistry 2024年第8期95卷 364-379页

作者： Xue Cai Caiping Zhang Zeping Chen Linjing Zhang Dirk Uwe Sauer Weihan Li National Active Distribution Network Technology Research Center Beijing Jiaotong University Chair for electrochemical energy Conversion and Storage Systems Institute for Power Electronics and Electrical Drives(ISEA) RWTH Aachen University Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems(CARL) Juelich Aachen Research Alliance JARA-Energy Helmholtz institute Münster(HI MS)

The safety and durability of lithium-ion batteries under mechanical constraints depend significantly on electrochemical, thermal, and mechanical fields in applications. Characterizing and quantifying the multi-field coupling behaviors requires interdisciplinary efforts. Here, we design experiments under mechanical constraints and introduce an in-situ analytical framework to clarify the complex interaction mechanisms and coupling degrees among multi-physics fields. The proposed analytical framework integrates the parameterization of equivalent models, in-situ mechanical analysis, and quantitative assessment of coupling behavior. The results indicate that the significant impact of pressure on impedance at low temperatures results from the diffusion-controlled step, enhancing kinetics when external pressure, like 180 to 240 k Pa at 10 °C, is applied. The diversity in control steps for the electrochemical reaction accounts for the varying impact of pressure on battery performance across different temperatures. The thermal expansion rate suggests that the swelling force varies by less than 1.60% per unit of elevated temperature during the lithiation process. By introducing a composite metric, we quantify the coupling correlation and intensity between characteristic parameters and physical fields, uncovering the highest coupling degree in electrochemical-thermal fields. These results underscore the potential of analytical approaches in revealing the mechanisms of interaction among multi-fields, with the goal of enhancing battery performance and advancing battery management.

关键词： Lithium-ion battery Muti-field coupling Mechanical constraints Interaction mechanisms Quantitative analysis

CFD-DEM simulation of fluorination reaction in fluidized beds with local grid and time refinement method

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Particuology 2024年第1期84卷 145-157页

作者： Mofan Qiu Lin Jiang Rongzhen Liu Yaping Tang Malin Liu institute of Nuclear and New energy Technology Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing100084China

The gas-solid reaction process with wide particle size distribution is extensively used in the chemical engineering field,especially the particle reacts with the gas gradually,such as fluorination reactions in fluidized beds.When the computational fluid dynamics-discrete element method(CFD-DEM)is used for the coupling simulation of multiphase and polydisperse particle reaction system,the grid size directly affects the accuracy of flow field information and simulation of chemical reaction.Furthermore,particle calculation time step will directly affect the efficiency of coupling calculation.In this work,a local grid and time step refinement method is proposed to simulate multiphase and polydisperse particle fluid-ization reaction system.In this method,the refined DEM grids are automatically generated in the computational domain around the fine particles,and the detailed fluid phase information is obtained with the interpolation algorithm.In the two-phase coupling process,particles are divided into different groups based on physical properties,each group has its own independent time step.The multistage conical-cylindrical spouted bed is proposed for the fluorination reaction process;the operating gas ve-locity range of the polydisperse particle system is extended by the new design while the particle size distribution changes with the gas-solid reaction process.It is demonstrated that the local grid and time step refinement method can improve the accuracy and efficiency of the traditional CFD-DEM method in the reaction process simulation,which describes a polydisperse particle system with wide particle size distribution.Aimed at improving the simulation accuracy and efficiency,this paper will be helpful for simulating the particle reaction process in the gas-solid fluidized bed and beneficial for the development of the CFD-DEM method.

关键词： CFD-DEM Polydisperse particle Two-phase flow Fluidized bed

CFD-DEM simulation of high density particles fluidization behaviors in 3D conical spouted beds

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Particuology 2024年第5期88卷 266-281页

作者： Lin Jiang Mofan Qiu Rongzheng Liu Bing Liu Youlin Shao Malin Liu institute of Nuclear and New energy Technology Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing 100084China

The spouted bed has been used in the coating process of high-density nuclear fuel particle.The particle fluidization behaviors in pseudo-2D and 3D spouted beds were simulated and validated.The effects of four independent variables(cone angle,particle density,inlet gas velocity,and particle loading)on particle fluidization behaviors in the 3D spouted bed were investigated systematically.The cone angle effect on fluidization mechanism was studied quantitatively first time.A new fluidization quality index was proposed based on the particle entrainment principle,and an extreme value was obtained when the cone angle was 60°,considered to be the optimum value for the 3D conical spouted bed.It was indicated the gas–solid contact efficiency can be kept up if the gas velocity was proportional toρp 0.65 and N p 0.78 when the particle density or loading was increased.These results will be useful for geometry and operation parameters design of the 3D conical spouted bed and helpful for developing the fluidization mechanism of high-density particles.

关键词： Spouted bed High-density particle CFD-DEM Fluidization quality index Particle loading

Magnetic-biased chiral molecules enabling highly oriented photovoltaic perovskites

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National Science Review 2024年第2期11卷 221-230页

作者： Jing Chen Caner Deger Zhen-Huang Su Kai-Li Wang Guang-Peng Zhu Jun-Jie Wu Bing-Chen He Chun-Hao Chen Tao Wang Xing-Yu Gao Ilhan Yavuz Yan-Hui Lou Zhao-Kui Wang Liang-Sheng Liao institute of Functional Nano&Soft Materials(FUNSOM) Laboratory of Advanced Negative Carbon TechnologiesSoochow University Department of Physics Marmara University Shanghai Synchrotron Radiation Facility(SSRF) Shanghai Advanced Research InstituteChinese Academy of Sciences College of energy Soochow Institute for Energy and Materials Innovations Soochow University Macao institute of Materials Science and Engineering Macau University of Science and Technology

The interaction between sites A, B and X with passivation molecules is restricted when the conventional passivation strategy is applied in perovskite（ABX3） photovoltaics. Fortunately, the revolving A-site presents an opportunity to strengthen this interaction by utilizing an external field. Herein, we propose a novel approach to achieving an ordered magnetic dipole moment, which is regulated by a magnetic field via the coupling effect between the chiral passivation molecule and the A-site（formamidine ion） in perovskites.This strategy can increase the molecular interaction energy by approximately four times and ensure a well-ordered molecular arrangement. The quality of the deposited perovskite film is significantly optimized with inhibited nonradiative recombination. It manages to reduce the open-circuit voltage loss of photovoltaic devices to 360 mV and increase the power conversion efficiency to 25.22%. This finding provides a new insight into the exploration of A-sites in perovskites and offers a novel route to improving the device performance of perovskite photovoltaics.

关键词： perovskite photovoltaics magnetic moment A-site regulation chiral molecules

Activatable photoacoustic bioprobe for visual detection of aging in vivo

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Chinese Chemical Letters 2024年第4期35卷 324-329页

作者： Zihong Li Jie Cheng Ping Huang Guoliang Wu Weiying Lin institute of Optical Materials and Chemical Biology Guangxi Key Laboratory of Electrochemical Energy MaterialsSchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Aging is a natural physiological process with various challenges, related to the loss of homeostasis within the organism, which is not a disease, but a significantly strong risk factor for multiple diseases, including myocardial infarction, stroke, some age-related cancers, macular degeneration, osteoarthritis, neurodegeneration, and many others. In the body, the main manifestation of aging is cellular aging, which exists within tissues and has a local or global impact on tissue function. However, the lack of effective aging detection tools has always been an issue that cannot be ignored in the field of aging research. Therefore,it is necessary to construct a non-invasive tool for in vivo detection of aging. Here, we show that the photoacoustic probe(LGAL), which has peak excitation and emission wavelengths in the near-infrared optical window, binds in vivo and at high contrast to the hallmark of aging, and allows for the microscopic imaging of aging through the intact mice. Firstly, this tool LGAL has been successfully applied to detect senescence in cells, displaying stronger photoacoustic signals than normal cells. Then, by using the photoacoustic probe, the blood vessels and tissues inside the mice can be visualized. Young and elderly mice exhibit varying intensities of photoacoustic signals, marking the first time a probe has been used to explore the aging of blood vessels and tissues inside the mice. Finally, we monitored the changes in the degree of aging during tumor treatment under photoacoustic(PA) imaging for the first time. As the treatment time increased, the degree of aging of the tumor gradually deepened. We expect the powerful tool could be a noninvasive and powerful tool for the study of aging biology.

关键词： Near-infrared Photoacoustic Aging Senescence Tumor Sa-β-gal