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Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries

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Nano-Micro Letters 2024年第5期16卷 370-383页

作者： Yu Du Weijie Chen Yu Wang Yue Yu Kai Guo Gan Qu Jianan Zhang Key Laboratory of advanced energy Catalytic and Functional Materials Preparation of Zhengzhou City College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001People’s Republic of China

Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in Li–S batteries.Spin selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions lead-ing to a significant reduction of the electronic repulsions in the orbitals of catalysts.Herein,we anchor the MgPc molecules on fluorinated carbon nanotubes(MgPc@FCNT),which exhibits the single active Mg sites with axial displacement.According to the density functional theory calculations,the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li–S batter-ies.As a result,the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^(-2) even when the high sulfur loading is 4.5 mg cm^(-2),and still maintains 5.1 mAh cm^(-2) after 100 cycles.This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li–S batteries.

关键词： Metal phthalocyanines Spin polarization Electrocatalysis Li–S batteries

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

Insight into demand-driven preparation of single-atomic mediators for lithium–sulfur batteries

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Journal of energy Chemistry 2024年第3期90卷 205-219,I0007页

作者： Miaoyu Lu Yifan Ding Zaikun Xue Ziang Chen Yuhan Zou Jingyu Sun college of energy Soochow Institute for Energy and Materials InnovationsKey Laboratory for Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina Beijing Graphene Institute Beijing 100095China

Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage systems.Strenuous efforts have been devoted to tackling the tremendous challenges,mainly pertaining to the severe shuttle effect,sluggish redox kinetics and lithium dendritic growth.Single-atomic mediators as promising candidates exhibit impressive performance in addressing these intractable issues.Related research often utilizes a trial-and-error approach,proposing solutions to fabricate single-atomic materials with diversified features.However,comprehensive review articles especially targeting demand-driven preparation are still in a nascent stage.Inspired by these considerations,this review summarizes the design of single-atomic mediators based on the application case-studies in LiS batteries and other metal-sulfur systems.Emerging preparation routes represented by chemical vapor deposition technology are introduced in a demand-oriented classification.Finally,future research directions are proposed to foster the advancement of single-atomic mediators in Li-S realm.

关键词： Single-atom catalyst Lithium–sulfur battery Chemical vapor deposition Demand-driven preparation

Homogenous coating of Li+ conductive Li5AlO4 on single-crystalline nonstoichiometric Li1.04Ni0.92Al0.04O2 for rechargeable lithium-ion batteries

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Journal of energy Chemistry 2024年第8期95卷 651-659页

作者： Guoyu Ding Shizhou Wang Jinhan Li Ziyan Wu Jiayu Chen Jiayong Du Xinhui Huang Kuiming Liu Yudong Zhang Zhonghan Wu Yiyang Peng Qiancheng Zhao Meng Yu Fangyi Cheng Key Laboratory of advanced energy Materials Chemistry(Ministry of Education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education) College of Chemistry Nankai University State Key Laboratory of advanced Chemical Power Sources Nankai University Haihe Laboratory of Sustainable Chemical Transformations

Cobalt-free,nickel-rich LiNi1-xAlxO2（x ≤ 0.1） is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance.In this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li5AlO4-coated single-crystalline slightly Li-rich Li1.04Ni0.92Al0.04O2.The symbiotic formation of Li5AlO4from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li5AlO4that permits high Li+conductivity.Benefiting from mitigated undesirable side reactions and phase evolution,the Li5AlO4-coated single-crystalline Li1.04Ni0.92Al0.04O2delivers a high specific capacity of220.2 mA h g-1at 0.1 C and considerable rate capability(182.5 mA h g-1at 10 C).Besides,superior capacity retention of 90.8% is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell.Furthermore,the particulate morphology of Li1.04Ni0.92Al0.04O2remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li0.98Ni0.97Al0.05O2features intragranular cracks and irreversible lattice distortion.The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

关键词： Aluminum segregation Cathode materials Molten synthesis Nonstoichiometric oxides Surface coating

Transfer-free chemical vapor deposition graphene for nitride epitaxy: challenges, current status and future outlook

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Science China Chemistry 2024年第3期67卷 824-840页

作者： Xiang Gao Senlin Li Jingfeng Bi Kaixuan Zhou Meng Li Zhongfan Liu Jingyu Sun college of energy Soochow Institute for Energy and Materials InnovationsSUDA-BGI Collaborative Innovation CenterKey Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006China Beijing Graphene Institute Beijing 100095China Xiamen Silan advanced Compound Semiconductor Co.Ltd. Xiamen 361026China

Graphene, a two-dimensional material with outstanding electrical and mechanical properties, has attracted considerable attention in the field of semiconductor technologies due to its potential use as a buffer layer for the epitaxial Ⅲ-nitride growth. In recent years, significant progress has been made in the chemical vapor deposition growth of graphene on various insulating substrates for the nitride epitaxy, which offers a facile, inexpensive, and easily scalable methodology. However, certain challenges are still present in the form of producing high-quality graphene and achieving optimal interface compatibility with Ⅲ-nitride materials.In this review, we provide an overview of the bottlenecks associated with the transferred graphene fabrication techniques and the state-of-the-art techniques for the transfer-free graphene growth. The present contribution highlights the current progress in the transfer-free graphene growth on different insulating substrates, including sapphire, quartz, SiO_(2)/Si, and discusses the potential applications of transfer-free graphene in the Ⅲ-nitride epitaxy. Finally, it includes the prospects of the transfer-free graphene growth for the Ⅲ-nitride epitaxy and the challenges that should be overcome to realize its full potential in this field.

关键词： Transfer-free chemical vapor deposition graphene for nitride epitaxy challenges current status and future outlook graphene

Self assembled electron blocking and lithiophilic interface towards dendrite-free solid-state lithium battery

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Chinese Chemical Letters 2024年第4期35卷 220-225页

作者： Caixia Li Yi Qiu Yufeng Zhao Wuliang Feng Institute for Sustainable energy&college of Sciences Shanghai UniversityShanghai 200444China Key Laboratory of advanced energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer from.Reducing the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable Li I interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li_7La_(3)Zr_(2)O_(12)(LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I_(2) thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm^(2) to 57 Ω/cm^(2). More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the Li I interphase, which leaded to a high critical current density of 1.2/7.0 m A/cm^(2) in the time/capacity-constant modes, respectively.

关键词： Li_7La_(3)Zr_(2)O_(12) LiI interphase Interfacial contact Li dendrite Thermodynamic stable

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

advanced organic electrode materials for aqueous rechargeable batteries

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Science China Chemistry 2024年第1期67卷 137-164页

作者： Gaojing Yang Yaxun Zhu Qi Zhao Zhimeng Hao Yong Lu Qing Zhao Jun Chen Frontiers Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China

Organic electrode materials take advantages of potentially sustainable production and structural tunability compared with present commercial inorganic electrode materials.However,their applications in traditional rechargeable batteries with nonaqueous electrolytes suffer from the premature failure and safety concerns.In comparison,aqueous rechargeable batteries based on organic electrode materials have received extensive attentions in recent years for low-cost and sustainable energy storage systems due to their inherent safety.This review aims to provide a comprehensive summary on the recent progress in advanced organic electrode materials for aqueous rechargeable batteries.We start from the overview of working principles and general design strategies of organic electrode materials in aqueous rechargeable batteries.Then the research advances of organic electrode materials in various aqueous rechargeable batteries are highlighted in terms of charge carriers(monovalent ions,multivalent ions,and anions).We emphasized the characteristics of organic electrode materials in various charge carriers.Finally,the critical challenges and future efforts of aqueous organic rechargeable batteries are discussed.More organic electrode materials with better electronic conductivity and fast reaction kinetics are still needed to build advanced aqueous batteries for commercial applications.

关键词： organic electrode materials aqueous batteries organic batteries rechargeable batteries

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