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PDOL-Based Solid Electrolyte Toward Practical Application:Opportunities and Challenges

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Nano-Micro Letters 2024年第7期16卷 109-141页

作者： Hua Yang Maoxiang Jing Li Wang Hong Xu Xiaohong Yan Xiangming He Institute for Advanced Materials School of Materials Science and EngineeringJiangsu UniversityZhenjiang 212013People’s Republic of China Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084People’s Republic of China

Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery assembly process are still the main challenges to hurdle the commercialization of SSLB.As the main component of SSLB,poly(1,3-dioxolane)(PDOL)-based solid polymer electrolytes polymerized in-situ are becoming a promising candidate solid elec-trolyte,for their high ion conductivity at room temperature,good battery elec-trochemical performances,and simple assembly process.This review analyzes opportunities and challenges of PDOL electrolytes toward practical application for polymer SSLB.The focuses include exploring the polymerization mechanism of DOL,the performance of PDOL composite electrolytes,and the application of PDOL.Furthermore,we provide a perspective on future research directions that need to be emphasized for commercialization of PDOL-based electrolytes in SSLB.The exploration of these schemes facilitates a comprehensive and profound understanding of PDOL-based polymer electrolyte and provides new research ideas to boost them toward practical application in solid-state batteries.

关键词： Poly(1,3-dioxolane) Solid electrolyte Polymerization mechanism Composite electrolyte Practical application

Tailoring Practically Accessible Polymer/Inorganic Composite Electrolytes for All-Solid-State Lithium Metal Batteries:A Review

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Nano-Micro Letters 2023年第3期15卷 266-297页

作者： Hongmei Liang Li Wang Aiping Wang Youzhi Song Yanzhou Wu Yang Yang Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084People’s Republic of China

Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.

关键词： Polymer Inorganic composite electrolytes All-solid-state lithium metal batteries Fillers Ionic conductivity High voltage

Functional Optical Fiber Sensors Detecting Imperceptible Physical/Chemical Changes for Smart Batteries

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NANO-MICRO LETTERS 2024年第1期16卷 1-41页

作者： Li, Yiding Wang, Li Song, Youzhi Wang, Wenwei Lin, Cheng he, xiangming Tsinghua Univ Inst Nucl & New Energy Technol Beijing 100084 Peoples R China Beijing Inst Technol BIT Natl Engn Res Ctr Elect Vehicles Beijing 100081 Peoples R China Natl Engn Res Ctr Elect Vehicles Shenzhen Automot Res Inst BIT Shenzhen Res Inst Shenzhen 518118 Peoples R China

Research progress of advanced optical fiber sensors in traction batteries and energy storage batteries is summarized.The embedded application mechanisms of different optical fiber sensors in batteries are discussed.Advanced optical fiber sensors adapting to batteries with diverse materials are reviewed.Advanced optical fiber sensors driving the development of future smart batteries are prospected. The battery technology progress has been a contradictory process in which performance improvement and hidden risks coexist. Now the battery is still a "black box", thus requiring a deep understanding of its internal state. The battery should "sense its internal physical/chemical conditions", which puts strict requirements on embedded sensing parts. This paper summarizes the application of advanced optical fiber sensors in lithium-ion batteries and energy storage technologies that may be mass deployed, focuses on the insights of advanced optical fiber sensors into the processes of one-dimensional nano-micro-level battery material structural phase transition, electrolyte degradation, electrode-electrolyte interface dynamics to three-dimensional macro-safety evolution. The paper contributes to understanding how to use optical fiber sensors to achieve "real" and "embedded" monitoring. Through the inherent advantages of the advanced optical fiber sensor, it helps clarify the battery internal state and reaction mechanism, aiding in the establishment of more detailed models. These advancements can promote the development of smart batteries, with significant importance lying in essentially promoting the improvement of system consistency. Furthermore, with the help of smart batteries in the future, the importance of consistency can be weakened or even eliminated. The application of advanced optical fiber sensors helps comprehensively improve the battery quality, reliability, and life.

关键词： Smart battery Advanced embedded optical fiber sensor Battery internal physical/chemical state Quality-reliability-life characteristic LITHIUM-ION BATTERY IN-SITU MEASUREMENTS STATE-OF-CHARGE REFRACTIVE-INDEX TheRMAL RUNAWAY LOW-TEMPERATURE STRAIN SENSOR LIQUID-LEVEL CELL STATE SAPPHIRE

Confining ultrafine Li3P nanoclusters in porous carbon for highperformance lithium-ion battery anode

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Nano Research 2020年第4期13卷 1122-1126页

作者： Eryang Mao Wenyu Wang Mintao Wan Li Wang Xiangming He Yongming Sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China

High-capacity lithium-containing alloy anodes(e.g.,Li4.4Si,Li4.4Sn,and Li3P)enable lithium-free cathodes(e.g.,Sulfur,V2O5,and FeF3)to produce next-generation lithium-ion batteries(LIBs)with high energy density.herein,we design a Li3P/C nanocomposite with Li3P ultrafine nanodomains embedded in micrometer-scale porous carbon particles.Benefiting from the unique micro/nanostructure of the Li3P/C nanocomposite,electrons transfer rapidly through the conductive pathway provided by the porous carbon framework and the volume change between Li3P and P is confined in the nanopores of the carbon,which avoids the collapse of the whole Li3P/C composite particles.As expected,the as-achieved Li3P/C nanocomposite provided a high available lithium-ion capacity of 791 mAh/g(calculated based on the mass of Li3P/C)at 0.1 C during the initial delithiation process.Meanwhile,the Li3P/C nanocomposite showed 75%of its 0.5 C capacity at 6 C and stable cycling stability.

关键词： Li3P nanoclusters porous carbon lithium-containing anode high capacity lithium-ion batteries

Perception of fundamental science to boost lithium metal anodes toward practical application

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Green Energy & Environment 2024年第3期9卷 454-472页

作者： Jinkun Wang Li Wang Hong Xu Li Sheng Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing100084China

As a key material for lithium metal batteries(LMBs),lithium metal is one of the most promising anode materials to break the bottleneck of battery energy density and a commonly used active material for reference electrodes.Although lithium anodes are regarded as the holy grail of lithium batteries,decades of exploration have not led to the successful commercialization of LMBs,due mainly to the challenges related to the inherent properties of lithium metal.To pave the way for further investigation,herein,a comprehensive review focusing on the fundamental science of lithium are provided.Firstly,the natures of lithium atoms and their isotopes,lithium clusters and lithium crystals are revisited,especially their structural and energetic properties.Subsequently,the electrochemical properties of lithium metal are reviewed.Numerous important concepts and scientific questions,including the electronic structure of lithium,influence of high pressure and low temperature on the properties of lithium,factors influencing lithium deposition,generation of lithium dendrites,and electrode potential of lithium in different electrolytes,are explained and analyzed in detail.Approaches to improve the performance of lithium anodes and thoughtfulness about the electrode potential in lithium battery research are proposed.

关键词： Lithium Cluster Crystal Physicochemical property Fundamental science

Molecular dynamics simulations of La_2O_3 thin films on SiO_2

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Journal of Energy Chemistry 2014年第3期23卷 282-286页

作者： Mou Fang Stephen P.Kelty Xiangming He Institute of Nuclear and New Energy Technology Tsinghua University State Key Laboratory of Automotive Safety and Energy Tsinghua University Huadong Institute of Lithium Ion Battery Department of Chemistry and Biochemistry Seton Hall University

Classical molecular dynamics is used to investigate the equilibrium state of the surface region and interface of heteroepitaxial La2O3 thin films.Due to the lattice mismatch,heteroepitaxial thin films are subject to very large stress.For this reason the behavior of La2O3 thin films at SiO2interface becomes an important concern.Our result indicates that La2O3 can uniformly wet SiO2 surface.The properties of the simulated films are analyzed and the lack of any discernible crystalline phase in epitaxial La2O3 on SiO2 indicates that the lattice mismatch between SiO2 and La2O3 is sufficiently large to prevent the formation of even short-range orders in La2O3 film.

关键词： molecular dynamics simulation heteroepitaxia thin film interface lattice mismatch equilibrium state

An evaluation of safety and survival for patients with locally advanced pancreatic cancer treated with irreversible electroporation combined with chemotherapy:a retrospectively observational study

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Journal of Pancreatology 2022年第1期5卷 27-35页

作者： Chaobin he Jun Wang Yize Mao xiangming Lao Shengping Li Department of Pancreatobiliary Surgery State Key L aboratory of Oncology in South ChinaCollaborative Innovation Center for Cancer MedicineSun Yat-sen University Cancer CenterGuangzhouGuangdong ProvinceChina

Objective:lreversible electroporation(IRE)is emerging as a new therapy for locally advanced pancreatic cancer(LAPC).We aimed to conduct survival and safety analyses in L APC patients after treatment with IRE combined with chemotherapy.Methods:A total of 64 patients with LAPC who had received IRE and chemotherapy were retrospectively collected from August 2015 to March 2019 at Sun Yat-sen University Cancer Center.Overall survival(OS)and progression-free survival(PFS)were evaluated using Kaplan-Meier method and compared by the log-rank test.A multivariate Cox regression model was used to determine the prognostic factors of survival.The perioperative complications of IRE were also evaluated.The study was approved by the Institutional Review Board of Sun Yat-sen University Cancer Center(approval No.C2021-003).Results:The median survival of all included patients were 24.63(95%confidence interval:21.78-27.49)for overall survival and 13.00(95%confidence inteval:8.81-17.19)months for progression-free survival,with 96.8%,51.9%,18.3%;and 52.3%,21.5%,7.9%as the 1-,2-and 3-year OS and PFS rates,respectively.Tumor size[OS,hazard ratio(HR)=1.768,P=0.048;PFS,HR=0.304,P=0.010],neoadjuvant chemotherapy(OS,HR=0338,P=0.030;PFS,HR=0.358,P=0.034),carbohydrate antigen 19-9 variation after IRE(OS,HR=19.320,P=0.003;PFS,HR=14.591,P=0.021)and tumor response after neoadjuvant chemotherapy(OS,HR-8.779,P=0.033;PFS,HR-5.562,P=0.008)were predictive factors of survival in patients with LAPC after IRE.Complications were observed in 20.3%of patients.Grade B pancreatic fistula was the most common complication.The complication rates of the late treatment group(6.1%)were significantly lower than those of the first 15 patients after IRE treatment(66.7%).The median length of hospital stay of late treatment group was 8.6days,which was also shorter than that of the early treatment group(10.0days).Conclusions:IRE combined with chemotherapy could improve survival of LAPC patients with acceptable complication rates.Therefore,it may be a suitable method for

关键词： Chemotherapy Efficacy lreversible electroporation Lcally advanoed pancreatic canoer Safety

Regulation voltage of LiNiPO_(4) by density functional theory(DFT)calculation to move towards practical application

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Interdisciplinary Materials 2023年第3期2卷 443-458页

作者： Bo Zhang Yufang he Aiping Wang Xiang Xiao Jinli Liu Yingqiang Wu Li Wang Hong Xu Jiangang Li Hao Zhang Xiangming He Institute of Nuclear&New Energy Technology Tsinghua UniversityBeijingChina College of Chemical Engineering Beijing University of Chemical TechnologyBeijingChina Beijing Key Laboratory of Advanced Chemical Energy Storage Technologies and Materials Research Institute of Chemical DefenseBeijingChina

LiNiPO_(4)(working at~5.1 V)shows potential advantages in the competition of cathode materials for lithium-ion batteries(LIBs)because of high energy density.However,the high-voltage electrolyte developed can only remain relatively stable in the range of less than 4.8V,so the operating voltage of LiNiPO_(4)needs to be adjusted to smaller to better exploit its high-voltage advantages.To regulate the operating voltage of LiNiPO_(4)while ensuring the relative stability of its electrochemical properties,in this work,all the 3d,4d,and 5d transition metals(TMs)are,respectively,doped into the Ni site of LiNiPO_(4)to screen out the doped models with excellent electrochemical performance.In particular,the changes in lattice structure,electronic properties,formation energy,mechanical properties,anisotropy,and working voltage were used as screening criteria.By considering the above screening criteria,the Cr-and Fe-doped LiNiPO_(4)with open circuit voltage~4.7 and~4.8 V are considered to have leading performance and can be used for applicable high-voltage LIBs.The screening results of this work can provide an overall understanding of the doping of LiNiPO_(4)by TMs and have advanced a theoretical idea for the design of new high-voltage LIBs cathode materials.

关键词： computational screening doping high voltage LiNiPO_(4) lithium-ion batteries

Boosting reversible charging of Li-ion batteries at low temperatures by a synergy of propylene carbonate-based electrolyte and defective graphite

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Nano Research 2024年第3期17卷 1491-1499页

作者： Yingqiang Wu Jiao Zhang Jinli Liu Li Sheng Bo Zhang Limin Wang Siqi Shi Li Wang Hong Xu Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences(CAS)Changchun 130022China China National Quality Supervision and Inspection Center for Industrial Explosive Materials Nanjing University of Science and TechnologyNanjing 210094China School of Materials Science and Engineering Materials Genome InstituteShanghai UniversityShanghai 200444China

Propylene carbonate(PC)-based electrolytes have exhibited significant advantages in boosting the low-temperature discharging of graphite-based Li-ion batteries.However,it is still unclear whether they can improve the charging property and suppress lithium plating.Studying this topic is challenging due to the problem of electrochemical compatibility.To overcome this issue,we introduced graphite with phase defects.The results show that the pouch-type full batteries using PC-based electrolyte exhibit steady performance over 500 cycles and can be reversibly charged over 30 times at-20℃ with an average Coulombic efficiency of 99.95%,while the corresponding value for the conventional ethylene carbonate(EC)-based electrolyte sample is only 31.20%.This indicates that the use of PC-based electrolyte significantly suppresses lithium plating during low-temperature charging.We further demonstrate that the improved performance is mainly attributed to the unique solvation structure,where PF-6more anions participate in solvation,leading to the formation of a stable F-rich solid state electrolyte interface on the graphite surface and a lower reduction tendency of Li+ions.This work inspires new ideas for the design of PC-based electrolytes for low-temperature charging and fast-charging batteries.

关键词： lithium-ion batteries graphite propylene carbonate low-temperature charging