4.5 Review

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

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JOURNAL OF MATERIALS CHEMISTRY A (2022)

Article Chemistry, Physical

Salt-solvent synchro-constructed robust electrolyte-electrode interphase for high-voltage lithium metal batteries

Mingming Fang et al.

Summary: This study reports an electrolyte design for high-voltage lithium metal batteries, which achieves stable operation and high capacity retention by constructing a thin yet robust inorganic-organic interlocking protective film.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

Article Chemistry, Physical

Stable lithium metal batteries enabled by localized high-concentration electrolytes with sevoflurane as a diluent

Caiyun Chang et al.

Summary: The study presents a localized high concentration electrolyte (LHCE) for high-voltage lithium batteries, using fluoromethyl 1,1,1,3,3,3-hexafluoroisopropyl ether (SFE) as a diluent in concentrated carbonate electrolyte. The optimized LHCE improves the wettability and conductivity of the electrolyte, resulting in dense and stable electrodeposition of Li metal and a robust solid-electrolyte interphase (SEI) layer. This leads to improved capacity retention and coulombic efficiency in Li||NMC811 cells.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

Article Chemistry, Physical

High cycle stability of Zn anodes boosted by an artificial electronic-ionic mixed conductor coating layer

Weijia Fan et al.

Summary: This study introduces an artificial mixed electronic-ionic conductive coating layer (Alg-Zn + AB@Zn) to address the issues of corrosion and dendrite growth in aqueous zinc ion batteries (ZIBs), resulting in improved cycle stability.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

Article Electrochemistry

A polymer electrolyte with a thermally induced interfacial ion-blocking function enables safety-enhanced lithium metal batteries

Huanrui Zhang et al.

Summary: Lithium metal batteries are considered one of the most promising energy storage systems due to their high capacity and low potential. However, safety issues caused by lithium dendrite growth and pulverization have limited their practical application. To address this, researchers have developed an in situ polymer electrolyte with thermally induced interfacial ion-blocking ability, resulting in improved safety and cyclability of lithium metal batteries.

ESCIENCE (2022)

Article Electrochemistry

Electroactive polymeric nanofibrous composite to drive in situ construction of lithiophilic SEI for stable lithium metal anodes

Ai-Long Chen et al.

Summary: A novel Li+ flux distributor achieved by placing PVDF/PMMA composite nanofiber interlayer on a current collector induces uniform lithium deposition to mitigate dendrite growth, improving the stability of lithium metal batteries. Experimental results show that the design enables molecular-level uniform Li nucleation, leading to high cycling stability and increased rate capacity.

ESCIENCE (2022)

Article Electrochemistry

Diluted High-Concentration Electrolyte Based on Phosphate for High-Performance Lithium-Metal Batteries

Mengchuang Liu et al.

Summary: A new diluted high concentration electrolyte (DHCE) containing lithium bis(fluorosulfonyl)imide, triethyl phosphate and fluorobenzene cosolvent has been developed, which greatly improves the cyclic efficiency and capacity retention of lithium metal batteries (LMBs), providing more possibilities for developing high-energy-density LMBs.

BATTERIES & SUPERCAPS (2022)

Article Materials Science, Multidisciplinary

Enhancing cycle stability of Li metal anode by using polymer separators coated with Ti-containing solid electrolytes

Zhao Yan et al.

Summary: The employment of Ti-containing solid electrolyte-coated separators greatly enhances the cycle performances of lithium metal anode in cells using liquid electrolytes, achieving more uniform lithium deposition and stable cycling in rechargeable lithium-ion batteries. The use of Ti-containing solid electrolytes modifies the anode and electrolyte interfacial properties, leading to improved homogeneity of lithium deposition.

RARE METALS (2021)

Article Nanoscience & Nanotechnology

Multifunctional Electrolyte Additive Stabilizes Electrode-Electrolyte Interface Layers for High-Voltage Lithium Metal Batteries

Yongchao Liu et al.

Summary: The use of N,O-bis(trimethylsilyl) trifluoro acetamide (BTA) as a multifunctional additive showed significant benefits in improving the electrochemical performance of lithium metal batteries, by modifying both anode and cathode surface layers. The BTA additive containing multiple functional groups promoted the formation of solid electrolyte interfacial films on a lithium metal anode and cathode surfaces, leading to enhanced electrode-electrolyte interfacial stability and reduced capacity decay caused by structural degradation of the cathode.

ACS APPLIED MATERIALS & INTERFACES (2021)

Article Chemistry, Multidisciplinary

Inhibiting Solvent Co-Intercalation in a Graphite Anode by a Localized High-Concentration Electrolyte in Fast-Charging Batteries

Li-Li Jiang et al.

Summary: By utilizing a localized high-concentration electrolyte, a uniform and robust solid electrolyte interphase can be achieved on the graphite surface, leading to fast-charging performance and excellent cycling stability of lithium-ion batteries.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

Article Multidisciplinary Sciences

Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries

Xia Cao et al.

Summary: The formulation and structure of electrolytes play a critical role in the performance of high-voltage Li metal batteries, with localized high-concentration electrolytes outperforming carbonate electrolytes in various aspects due to their unique solvation structures.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2021)

Article Chemistry, Multidisciplinary

Design of a LiF-Rich Solid Electrolyte Interphase Layer through Highly Concentrated LiFSI-THF Electrolyte for Stable Lithium Metal Batteries

Thuy Duong Pham et al.

Summary: A highly concentrated LiFSI-THF electrolyte system has been introduced, allowing for high CE cycling of lithium metal anodes without dendrite growth. The excellent charge-discharge performance is attributed to the increased cation-anion associated complexes in the electrolyte.
Article Chemistry, Physical

How Does External Pressure Shape Li Dendrites in Li Metal Batteries?

Xin Shen et al.

Summary: External pressure has a significant impact on the morphology and performance of Li metal batteries, affecting the electroplating reactions and the shape of dendrites. A phase diagram of routine electrolytes under various external pressures has been established, providing rational guidance for designing pressure management systems in batteries.

ADVANCED ENERGY MATERIALS (2021)

Article Multidisciplinary Sciences

Rational design of mechanically robust Ni-rich cathode materials via concentration gradient strategy

Tongchao Liu et al.

Summary: The study found that using concentration gradient design can successfully alleviate particle cracking issues in Ni-rich cathode materials without sacrificing electrode capacity. By investigating the effects of Co and Mn on the mechanical properties of Ni-rich materials, it is found that Co-enriched surface design helps suppress particle cracking formation, while Mn-enriched core limits internal expansion and improves structural integrity. The concentration gradient design also promotes morphological stability and cycling performances in Li metal coin cell configuration.

NATURE COMMUNICATIONS (2021)

Article Engineering, Chemical

Stable interfaces constructed by concentrated ether electrolytes to render robust lithium metal batteries

He Liu et al.

Summary: By forming a stable solid electrolyte interphase on the Li metal surface, the interface between high-voltage cathodes and anodes in lithium metal batteries has been improved, resulting in enhanced cycle life and capacity retention of the battery.

CHINESE JOURNAL OF CHEMICAL ENGINEERING (2021)

Article Chemistry, Physical

Improving Cycling Stability of Vanadium Sulfide (VS4) as a Li Battery Cathode Material Using a Localized High-Concentration Carbonate-Based Electrolyte

Yuta Maeyoshi et al.

Summary: A localized high-concentration electrolyte is reported in this study, which can stabilize Li metal anodes, improve the Coulombic efficiency and cycling stability of the cathode. By inhibiting the dissolution of V from VS4 and forming a LiF-rich layer, the degradation of the cathode is effectively suppressed.

ACS APPLIED ENERGY MATERIALS (2021)

Article Chemistry, Multidisciplinary

Simultaneous Stabilization of the Solid/Cathode Electrolyte Interface in Lithium Metal Batteries by a New Weakly Solvating Electrolyte

Thuy Duong Pham et al.

Summary: The study introduces 1,2-diethoxyethane (DEE) as a new electrolytic solvent for lithium metal batteries (LMBs), which shows improved cycling stability and Coulombic efficiencies. The use of DEE helps in reducing dendrite growth, preventing unwanted side-reactions, and creating possibilities for high-energy-density rechargeable LMBs.
Article Chemistry, Physical

Intrinsically Nonflammable Ionic Liquid-Based Localized Highly Concentrated Electrolytes Enable High-Performance Li-Metal Batteries

Zhicheng Wang et al.

Summary: An intrinsically nonflammable ionic liquid-based localized highly concentrated electrolyte (LHCE) has been designed, which significantly improves the performance of Li-metal batteries (LMBs) by enhancing ionic conductivity and suppressing Li dendrite growth. The LHCE exhibits high Coulombic efficiency and stable cycling performance over thousands of cycles, making it suitable for various LMB systems. This electrolyte shows great potential for practical application in high-performance batteries.

ADVANCED ENERGY MATERIALS (2021)

Article Nanoscience & Nanotechnology

Understanding the Effects of the Low-Concentration Electrolyte on the Performance of High-Energy-Density Li-S Batteries

Jicheng Jiang et al.

Summary: A new method protocol was proposed to investigate the effects of low-concentration electrolytes on the cathode and anode for Li-S batteries separately. It was found that 0.5M LiTFSI exhibited better cycling stability under high sulfur loading conditions, and the low-concentration electrolyte could improve the stability of the Li-electrolyte interface. This was attributed to a higher organic component content in the SEI, allowing for better accommodation of volume changes in the Li metal anode.

ACS APPLIED MATERIALS & INTERFACES (2021)

Article Chemistry, Multidisciplinary

Double Ionic-Electronic Transfer Interface Layers for All-Solid-State Lithium Batteries

Jingang Zheng et al.

Summary: This study successfully reduced the interface resistance of solid-state lithium batteries by growing double ionic-electronic transfer interface layers at the electrode-electrolyte interfaces, achieving higher cycling stability and charge-discharge efficiency.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

Article Chemistry, Physical

A Multifunctional Dual-Salt Localized High-Concentration Electrolyte for Fast Dynamic High-Voltage Lithium Battery in Wide Temperature Range

Shuangshuang Lin et al.

Summary: This study introduces a multifunctional high-concentration electrolyte containing fluorocarbonate, which shows excellent performance under high voltage and low temperature conditions, providing a new approach for designing high-performance lithium batteries.

ADVANCED ENERGY MATERIALS (2021)

Article Chemistry, Physical

Enhancing the Cycling Stability for Lithium-Metal Batteries by Localized High-Concentration Electrolytes with 2-Fluoropyridine Additive

Qian Wu et al.

Summary: This study investigates the cycling stability of Li-metal anode in various electrolytes, with the finding that the system of LHCE + 2-FP exhibits the best performance, including the longest stable cycle time and highest coulombic efficiency.

ACS APPLIED ENERGY MATERIALS (2021)

Review Multidisciplinary Sciences

Comparative performance of ex situ artificial solid electrolyte interphases for Li metal batteries with liquid electrolytes

Francesca Lorandi et al.

Summary: The study reviewed the use of artificial solid electrolyte interphases in high-energy Li metal batteries, emphasizing the importance of testing conditions aligned with practical battery systems.

ISCIENCE (2021)

Review Chemistry, Multidisciplinary

Mechanism understanding for stripping electrochemistry of Li metal anode

Feng-Ni Jiang et al.

Summary: This review critically examines the current research status on the stripping electrochemistry of lithium metal anode, emphasizing the importance of the stripping process for robust lithium metal anode. The factors affecting stripping processes and corresponding solutions are summarized and categorized, offering fresh insights for exploring lithium anode and designing robust lithium metal batteries based on comprehensive understanding of the stripping electrochemistry.

SUSMAT (2021)

Article Chemistry, Physical

Influence of diluent concentration in localized high concentration electrolytes: elucidation of hidden diluent-Li+ interactions and Li+ transport mechanism

Saul Perez Beltran et al.

Summary: Localized high concentration electrolytes (LHCE) serve as a feasible dilution strategy for high concentration electrolytes (HCE) to lower viscosity and increase ionic conductivity; TTE competes with Li+ for reactions, altering the reductive/oxidative behavior of the electrolyte.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

Article Materials Science, Multidisciplinary

New Insights on the Good Compatibility of Ether-Based Localized High-Concentration Electrolyte with Lithium Metal

Tao Li et al.

Summary: This study conducted a systematic comparison between two representative high-concentration electrolytes (LHCEs) based on DMC and DME in high-voltage Li metal batteries, revealing that DME-based LHCE exhibits better compatibility and stability with Li metal anodes than DMC-based LHCE. The findings provide fresh insights on the stable nature of ether-based LHCE with Li metal anodes for advanced electrolyte engineering.

ACS MATERIALS LETTERS (2021)

Article Materials Science, Multidisciplinary

A binary PMMA/PVDF blend film modified substrate enables a superior lithium metal anode for lithium batteries

Xiaosong Xiong et al.

Summary: A thin PMMA/PVDF gel coating prepared on a Cu substrate directly improves the cycling performance of lithium metal anodes, enhances the stability of the electrode interface, and achieves stable cycling for over 1400 hours.

MATERIALS ADVANCES (2021)

Article Chemistry, Physical

Formation mechanism of the solid electrolyte interphase in different ester electrolytes

Shi-Jie Yang et al.

Summary: The formation mechanisms of SEI in electrolytes with DEC and EC were studied, revealing that LEC can disperse in the electrolyte while LEDC cannot. First-principles calculations confirmed that the low polymerization degree of LEC leads to its good dispersity, while poly-LEDC can remain on the Li surface as the stable SEI.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

Article Chemistry, Multidisciplinary

A perspective on sustainable energy materials for lithium batteries

Xin-Bing Cheng et al.

Summary: Lithium-ion batteries have been successful in portable electronics and electric vehicles, but face challenges in terms of sustainable development, requiring innovation in material chemistry and safety performance, as well as the importance of battery recycling for a sustainable society.

SUSMAT (2021)

Article Chemistry, Multidisciplinary

Electrolyte and anode-electrolyte interphase in solid-state lithium metal polymer batteries: A perspective

Heng Zhang et al.

Summary: The interest in solid-state lithium metal batteries, utilizing solid polymer electrolytes, has been growing due to their higher energy density and improved safety. Research focuses on improving the ionic conductivity of SPEs and their interface stability with lithium anodes, as well as exploring advanced characterizing techniques for in-depth understanding of the battery interphases.

SUSMAT (2021)

Review Electrochemistry

Review-Localized High-Concentration Electrolytes for Lithium Batteries

Xia Cao et al.

Summary: Conventional LiPF6/carbonate-based electrolytes have been widely used in graphite-based lithium ion batteries for their stability, but are less stable in Li metal and silicon anodes. Localized high-concentration electrolytes have unique advantages, forming stable SEI layers to improve stability.

JOURNAL OF THE ELECTROCHEMICAL SOCIETY (2021)

Article Nanoscience & Nanotechnology

Three-Dimensional Superlithiophilic Interphase for Dendrite-Free Lithium Metal Anodes

Yun Qiao et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

Article Nanoscience & Nanotechnology

Cycling Performance and Kinetic Mechanism Analysis of a Li Metal Anode in Series-Concentrated Ether Electrolytes

Simin Wang et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

Article Nanoscience & Nanotechnology

Stable Cycling of High-Voltage Lithium-Metal Batteries Enabled by High-Concentration FEC-Based Electrolyte

Wei Wang et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

Article Nanoscience & Nanotechnology

Highly Conductive Polymeric Ionic Liquid Electrolytes for Ambient-Temperature Solid-State Lithium Batteries

Fengrui Zhang et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

Article Chemistry, Multidisciplinary

High-Safety and High-Energy-Density Lithium Metal Batteries in a Novel Ionic-Liquid Electrolyte

Hao Sun et al.

ADVANCED MATERIALS (2020)

Article Chemistry, Multidisciplinary

Fluorinated Aromatic Diluent for High-Performance Lithium Metal Batteries

Dong-Joo Yoo et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

Article Nanoscience & Nanotechnology

Functional Localized High-Concentration Ether-Based Electrolyte for Stabilizing High-Voltage Lithium-Metal Battery

Shuangshuang Lin et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

Article Chemistry, Multidisciplinary

Homogeneous and Fast Ion Conduction of PEO-Based Solid-State Electrolyte at Low Temperature

Shengjun Xu et al.

ADVANCED FUNCTIONAL MATERIALS (2020)

Article Chemistry, Multidisciplinary

Lithium Nitrate Regulated Sulfone Electrolytes for Lithium Metal Batteries

Jiale Fu et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

Article Multidisciplinary Sciences

Thermal runaway of Lithium-ion batteries employing LiN(SO2F)2-based concentrated electrolytes

Junxian Hou et al.

NATURE COMMUNICATIONS (2020)

Article Multidisciplinary Sciences

Role of inner solvation sheath within salt-solvent complexes in tailoring electrode/electrolyte interphases for lithium metal batteries

Xiaodi Ren et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2020)

Article Chemistry, Multidisciplinary

High-Energy Rechargeable Metallic Lithium Battery at-70°C Enabled by a Cosolvent Electrolyte

Xiaoli Dong et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019)

Article Chemistry, Physical

High-Concentration Ether Electrolytes for Stable High-Voltage Lithium Metal Batteries

Xiaodi Ren et al.

ACS ENERGY LETTERS (2019)

Article Nanoscience & Nanotechnology

Long-Term Stable Lithium Metal Anode in Highly Concentrated Sulfolane-Based Electrolytes with Ultrafine Porous Polyimide Separator

Yuta Maeyoshi et al.

ACS APPLIED MATERIALS & INTERFACES (2019)

Article Chemistry, Multidisciplinary

Electrochemical Diagram of an Ultrathin Lithium Metal Anode in Pouch Cells

Peng Shi et al.

ADVANCED MATERIALS (2019)

Article Chemistry, Physical

Lithium metal batteries capable of stable operation at elevated temperature

Zhen Geng et al.

ENERGY STORAGE MATERIALS (2019)

Article Electrochemistry

Improved Stability and Rate Capability of Ionic Liquid Electrolyte with High Concentration of LiFSI

Ashley Heist et al.

JOURNAL OF THE ELECTROCHEMICAL SOCIETY (2019)

Article Chemistry, Physical

Localized high concentration electrolyte behavior near a lithium-metal anode surface

Yu Zheng et al.

JOURNAL OF MATERIALS CHEMISTRY A (2019)

Article Chemistry, Multidisciplinary

High-Voltage Lithium-Metal Batteries Enabled by Localized High-Concentration Electrolytes

Shuru Chen et al.

ADVANCED MATERIALS (2018)

Article Chemistry, Multidisciplinary

A highly concentrated phosphate-based electrolyte for high-safety rechargeable lithium batteries

Pengcheng Shi et al.

CHEMICAL COMMUNICATIONS (2018)

Article Nanoscience & Nanotechnology

Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries

Xiulin Fan et al.

NATURE NANOTECHNOLOGY (2018)

Article Energy & Fuels

Stable cycling of high-voltage lithium metal batteries in ether electrolytes

Shuhong Jiao et al.

NATURE ENERGY (2018)

Article Nanoscience & Nanotechnology

Wide-Temperature Electrolytes for Lithium-Ion Batteries

Qiuyan Li et al.

ACS APPLIED MATERIALS & INTERFACES (2017)

Article Chemistry, Multidisciplinary

Anode-Free Rechargeable Lithium Metal Batteries

Jiangfeng Qian et al.

ADVANCED FUNCTIONAL MATERIALS (2016)

Article Multidisciplinary Sciences

Superconcentrated electrolytes for a high-voltage lithium-ion battery

Jianhui Wang et al.

NATURE COMMUNICATIONS (2016)

Article Chemistry, Multidisciplinary

Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy

Kevin N. Wood et al.

ACS CENTRAL SCIENCE (2016)

Review Chemistry, Multidisciplinary

Rational material design for ultrafast rechargeable lithium-ion batteries

Yuxin Tang et al.

CHEMICAL SOCIETY REVIEWS (2015)

Review Electrochemistry

Review-Superconcentrated Electrolytes for Lithium Batteries

Yuki Yamada et al.

JOURNAL OF THE ELECTROCHEMICAL SOCIETY (2015)

Article Multidisciplinary Sciences

High rate and stable cycling of lithium metal anode

Jiangfeng Qian et al.

NATURE COMMUNICATIONS (2015)

Article Chemistry, Multidisciplinary

Concentrated electrolytes: decrypting electrolyte properties and reassessing Al corrosion mechanisms

Dennis W. McOwen et al.

ENERGY & ENVIRONMENTAL SCIENCE (2014)

Review Chemistry, Multidisciplinary

Lithium metal anodes for rechargeable batteries

Wu Xu et al.

ENERGY & ENVIRONMENTAL SCIENCE (2014)

Article Chemistry, Multidisciplinary

A superconcentrated ether electrolyte for fast-charging Li-ion batteries

Yuki Yamada et al.

CHEMICAL COMMUNICATIONS (2013)

Article Chemistry, Multidisciplinary

The Li-Ion Rechargeable Battery: A Perspective

John B. Goodenough et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2013)

Article Chemistry, Multidisciplinary

New Nanostructured Li2S/Silicon Rechargeable Battery with High Specific Energy

Yuan Yang et al.

NANO LETTERS (2010)