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Localized high-concentration electrolytes for lithium metal batteries:progress and prospect

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Frontiers of Chemical Science and Engineering 2023年第10期17卷 1354-1371页

作者： Jia-xin Guo Wen-Bo Tang Xiaosong Xiong He Liu Tao Wang Yuping Wu xin-bing cheng School of Energy and Environment Southeast UniversityNanjing 211189China School of Chemistry and Materials Science Nanjing University of Information Science and TechnologyNanjing 210044China

With the increasing development of digital devices and electric vehicles,high energy-density rechargeable batteries are strongly *** one of the most promising anode materials with an ultrahigh specific capacity and extremely low electrode potential,lithium metal is greatly considered an ideal candidate for nextgeneration battery ***,limited Coulombic efficiency and potential safety risks severely hinder the practical applications of lithium metal batteries due to the inevitable growth of lithium dendrites and poor interface *** efforts have been explored to address these challenges,mainly focusing on the design of novel ***,we provide an overview of the recent developments of localized high-concentration electrolytes in lithium metal ***,the solvation structures and physicochemical properties of localized high-concentration electrolytes are ***,the developments of localized high-concentration electrolytes to suppress the formation of dendritic lithium,broaden the voltage window of electrolytes,enhance safety,and render low-temperature operation for robust lithium metal batteries are ***,the remaining challenges and further possible research directions for localized highconcentration electrolytes are outlined,which can promisingly render the practical applications of lithium metal batteries.

关键词： high-concentration electrolyte localized high-concentration electrolyte lithium metal battery solid electrolyte interphase dendrite

Dendrite-free sandwiched ultrathin lithium metal anode with even lithium plating and stripping behavior

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Nano Research 2019年第9期12卷 2224-2229页

作者： Tao Li Peng Shi Rui Zhang He Liu xin-bing cheng Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Thin artificial solid electrolyte coatings are effective to enhance the electrochemical performances and safety issues of lithium (Li) metal ***,massive and efficient fabrication of artificial protection layers on Li metal anode surface remains ***,we describe a sandwiched Li metal anode fabricated through a continuous roll to roll calendering method to implant a thin and large-area carbon layer on Li metal anode surface at room ***,a carbon layer (~ 3 μm in thickness) can be entirely grafted from Cu substrate to 50 pm Li belt surface due to the stickiness of metallic *** carbon layer not only plays a critical role in providing rich nucleation sites for Li plating,but more importantly diminishes the metallurgical nonuniformity effects (slip lines) on ***,even Li plating/stripping morphologies are achieved and the as-obtained sandwiched Li/C composite anodes exhibit improved cycling stability both in Li | LiFePO4 and Li | S coin cells and pouch *** continuous roll to roll calendering strategy opens a new avenue for grafting various thin artificial protection layers on Li metal surface for safe rechargeable batteries.

关键词： lithium metal anodes artificial solid electrolyte in terphases carb on nano materials Li strippi ng/plating rechargeable batteries

Plating current density distribution of lithium metal anodes in pouch cells

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Journal of Energy Chemistry 2022年第6期31卷 70-75,I0003页

作者： Shi-Jie Yang xin Shen xin-bing cheng Feng-Ni Jiang Rui Zhang He Liu Lei Liu Hong Yuan School of Materials Science&Engineering Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 211189JiangsuChina School of Chemistry and Materials Science Nanjing University of Information Science&TechnologyNanjing 210044JiangsuChina Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina

The uniformity of current density distribution upon electrodes is one of the most important factors determining the lithium dendrites growth and cycling performance of lithium metal batteries(LMBs). Herein,current density distributions of lithium metal anodes induced by various engineering factors, consisting of uneven cathode, electrolyte distribution, and different tab positions, and their effects on the electrochemical performance are investigated theoretically and experimentally in pouch cells. The deviation of current density in lithium metal anodes ranges from 2.47% to 196.18% due to the different levels of uneven cathode materials. However, the deviation is just 13.60% for different electrolyte thicknesses between cathodes and anodes, even a ten-layer separator in some positions. The maximum deviation for variational tab positions is only 0.17%. The nonuniformity in current density distribution results in severe dendrite growth issues and poor electrochemical performance of LMBs. This work not only confirms the direct correlation between the uneven current density distribution and lithium deposition behaviors, but also points out the decisive effects of cathode surface roughness on current distribution of anodes, to which more attentions should be paid in practical applications of LMBs.

关键词： Pouch cell Lithium metal anode Dendrite Current density distribution Safety

Favorable Lithium Nucleation on Lithiophilic Framework Porphyrin for Dendrite-Free Lithium Metal Anodes

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Research 2019年第1期2019卷 1249-1259页

作者： Bo-Quan Li Xiao-Ru Chen Xiang Chen Chang-xin Zhao Rui Zhang xin-bing cheng Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Lithium metal constitutes promising anode materials but sufers from dendrite *** host materials are highly considered for achieving uniform lithium *** construction of lithiophilic sites with desired structure and homogeneous distribution signifcantly promotes the lithiophilicity of lithium hosts but remains a great *** this contribution,a framework porphyrin(POF)material with precisely constructed lithiophilic sites in regard to chemical structure and geometric position is employed as the lithium host to address the above issues for dendrite-free lithium metal *** extraordinary lithiophilicity of POF even beyond lithium nuclei validated by DFT simulations and lithium nucleation overpotentials afords a novel mechanism of favorable lithium nucleation to facilitate uniform nucleation and inhibit dendrite ***,POF-based anodes demonstrate superior electrochemical performances with high Coulombic efciency over 98%,reduced average voltage hysteresis,and excellent stability for 300 cycles at 1.0 mA cm^(−2),1.0 mAh cm^(−2) superior to both Cu and graphene *** favorable lithium nucleation mechanism on POF materials inspires further investigation of lithiophilic electrochemistry and development of lithium metal batteries.

关键词： lithium POF hysteresis

A perspective on sustainable energy materials for lithium batteries

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SusMat 2021年第1期1卷 38-50页

作者： xin-bing cheng He Liu Hong Yuan Hong-Jie Peng cheng Tang Jia-Qi Huang Qiang Zhang Department of Chemical Engineering Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyTsinghua UniversityBeijingP.R.China Advanced Research Institute for Multidisciplinary Science Beijing Institute of TechnologyBeijingP.R.China Department of Chemical Engineering Stanford UniversityStanfordCaliforniaUSA School of Chemical Engineering and Advanced Materials University of AdelaideAdelaideSouth AustraliaAustralia

Lithium ion battery has achieved great success in portable electronics and even recently electronic vehicles since its commercialization in ***,lithium-ion batteries are confronted with several issues in terms of the sustainable development such as the high price of raw materials and electronic products,the emerging safety accidents,*** recent progresses are herein emphasized on lithium batteries for energy storage to clearly understand the sustainable energy chemistry and emerging *** Perspective presents novel lithium-ion batteries developed with the aims of enhancing the electrochemical performance and sustainability of energy storage ***,revolutionary material chemistries,including novel low-cobalt cathode,organic electrode,and aqueous electrolyte,are ***,the characteristics of safety performance are analyzed and strategies to enhance safety are subsequently *** recycling is considered as the key factor for a sustainable society and related technologies are present as ***,conclusion and outlook are drawn to shed lights on the further development of sustainable lithium-ion batteries.

关键词： aqueous batteries battery recycling lithium batteries organic cathode safety sustainable energy materials

Inherent thermal-responsive strategies for safe lithium batteries

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Journal of Energy Chemistry 2024年第2期89卷 519-534,I0012页

作者： Jia-xin Guo Chang Gao He Liu Feng Jiang Zaichun Liu Tao Wang Yuan Ma Yiren Zhong Jiarui He Zhi Zhu Yuping Wu xin-bing cheng School of Energy and Environment Southeast UniversityNanjing 211189JiangsuChina School of Chemistry and Materials Science Nanjing University of Information Science and TechnologyNanjing 210044JiangsuChina

Safe batteries are the basis for next-generation application scenarios such as portable energy storage devices and electric vehicles,which are crucial to achieving carbon ***,separators,and electrodes as main components of lithium batteries strongly affect the occurrence of safety *** materials,which can respond to external stimuli or environmental change,have triggered extensive attentions recently,holding great promise in facilitating safe and smart *** review thoroughly discusses recent advances regarding the construction of high-safety lithium batteries based on internal thermal-responsive strategies,together with the corresponding changes in electrochemical performance under external ***,the existing challenges and outlook for the design of safe batteries are presented,creating valuable insights and proposing directions for the practical implementation of safe lithium batteries.

关键词： Lithium battery Thermal safety Thermal runaway Thermal-responsive

Dual-layer vermiculite nanosheet based hybrid film to suppress dendrite growth in lithium metal batteries

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Journal of Energy Chemistry 2022年第6期31卷 205-210,I0006页

作者： Xiang-Qun Xu Feng-Ni Jiang Shi-Jie Yang Ye Xiao He Liu Fangyang Liu Lei Liu xin-bing cheng Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 211189JiangsuChina School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina School of Chemistry and Materials Science Nanjing University of Information Science&TechnologyNanjing 210044JiangsuChina Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina

Lithium metal anode has become a favorable candidate for next-generation rechargeable ***, the unstable interface between lithium metal and electrolyte leads to the growth of dendrites,resulting in the low Coulombic efficiency and even the safety concerns. Herein, a rigid-flexible dual-layer vermiculite nanosheet(VN) based organic-inorganic hybrid film on lithium metal anode is proposed to suppress dendrite growth and relieve volume fluctuations. The inner mechanically robust VN layer(3 μm thick) enhances the mechanical properties of the protective layer, while the outer polymer(4 μm thick) can enhance the flexibility of the hybrid layer. The Li | Li symmetric cell with protected lithium shows an extended life of over 670 h. The full cell with Li anode protected by dual-layer interface exhibits a better capacity retention of 80% after 174 cycles in comparison to bare Li anode with 94 *** study provides a novel approach and a significant step towards prolonging lifespan of lithium metal batteries.

关键词： Lithium metal anode Dendrite Organic-inorganic hybrid layer Dual-layer interface Two-dimensional vermiculite nanosheet

A two-dimension laminar composite protective layer for dendrite-free lithium metal anode

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Journal of Energy Chemistry 2021年第5期30卷 391-394页

作者： Xiang-Qun Xu Rui Xu xin-bing cheng Ye Xiao Hong-Jie Peng Hong Yuan Fangyang Liu School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Department of Chemical Engineering Stanford UniversityStanfordCA 94305 USA

Lithium(Li)metal anodes with the high theoretical specific capacity(3860 mAh g^(-1))and most negative reduction potential(-3.04 V *** hydrogen electrode)have been considered as an ultimate choice for energy storage devices with high energy density[1-4].However,the practical applications of Li metalbased batteries(LMBs)are confronted with two tough issues:Li dendrite growth induced by uneven Li depositions and unstable solid electrolyte interphase(SEI)(Fig.1a)[5,6].

关键词： Lithium metal anode Artificial protective layer 2D materials Vermiculite sheets Laminar arrangement

Higher-order polysulfides induced thermal runaway for 1.0 Ah lithium sulfur pouch cells

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Particuology 2023年第8期79卷 10-17页

作者： Feng-Ni Jiang Shi-Jie Yang Zi-Xian Chen He Liu Hong Yuan Lei Liu Jia-Qi Huang xin-bing cheng Qiang Zhang College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan030024ShanxiChina Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing211189JiangsuChina School of Chemistry and Materials Science Nanjing University of Information Science and TechnologyNanjing210044JiangsuChina

Comprehensive analyses on thermal runaway mechanisms are critically vital to achieve the safe lithium-sulfur(Li-S)*** reactions between dissolved higher-order polysulfides and Li metal were found to be the origins for the thermal runaway of 1.0 Ah cycled Li-S pouch cells.16-cycle pouch cell indicates high safety,heating from 30 to 300 ℃ without thermal runaway,while 16-cycle pouch cell with additional electrolyte undergoes severe thermal runaway at 147.9 ℃,demonstrating the key roles of the electrolyte on the thermal safety of *** the contrary,thermal runaway does not occur for 45-cycle pouch cell despite the addition of the *** is found that the higher-order polysulfides(Li_(2)S_(x) ≥ 6)are discovered in 16-cycle electrolyte while the sulfur species in 45-cycle electrolyte are Li_(2)S_(x) ≤ *** addition,strong exothermic reactions are discovered between cycled Li and dissolved higher-order polysulfide(Li_(2)S_(6) and Li_(2)S_(8))at 153.0 ℃,driving the thermal runaway of cycled Li-S pouch *** work uncovers the potential safety risks of Li-S batteries and negative roles of the polysulfide shuttle for Li-S batteries from the safety view.

关键词： Lithium-sulfur batteries Thermal runaway Polysulfides Pouch cell Polysulfide shuttle