Unravelling the convoluted and dynamic interphasial mechanisms on Li metal anodes

Tan, Sha; Kim, Ju‐Myung; Corrao, Adam A.; Ghose, Sanjit; Zhong, Hui; Rui, Ning; Wang, Xuelong; Senanayake, Sanjaya D.; Polzin, Bryant J.; Khalifah, Peter G.; Xiao, Jie; Liu, Jun; Xu, Ke; Yang, Xiao‐Qing; Cao, Xia; Hu, Enyuan

doi:10.1038/s41565-022-01273-3

Cited by 47 publications

(36 citation statements)

References 31 publications

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“…The distribution of Ni elements during the reversible plating/stripping process was further studied through time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS) analysis (Figure 5d,e). [ 1d,28 ] The Ni − signals of the undecorated sample show a high density of counts across the entire surface. On the contrary, the secondary ion signals of the M‐E@Celgard assisting anode become weak, which is contributed by the suppression of TM‐ions crosstalk.…”

Section: Resultsmentioning

confidence: 99%

“…Lithium metal batteries (LMBs) with high‐voltage (HV) cathodes and Li anodes have been pursued as the “Holy Grail” for high‐energy‐density rechargeable batteries. [ 1 ] Obviously, the fascinating theoretical specific capacity (3860 mA h g −1 ) and the lowest reduction potential (−3.04 V versus standard hydrogen electrode) allow Li to be the best anode candidate. [ 2 ] For cathode materials, Ni‐rich layered oxides LiNi x Co y Mn 1– x – y O 2 ( x > 0.5, NCM) have received great attention by the virtue of their inspiring output capacity and voltage.…”

Section: Introductionmentioning

confidence: 99%

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Taming Active‐Ion Crosstalk by Targeted Ion Sifter Toward High‐Voltage Lithium Metal Batteries

Feng,

Zhong,

Zhang

et al. 2023

Advanced Energy Materials

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Lithium metal batteries (LMBs), based on high‐voltage (HV) LiNixCoyMnzO2 (NCM, x+y+z = 1) materials, exhibit great potential for next‐generation electric vehicle (EV) cells. Nevertheless, the inevitable dissolution and shuttle of transition metal (TM) ions from NCM cathodes poses a threat to the electrochemical sustainability of LMBs, especially at high voltage and high temperatures. Herein, ethylene diamine tetraacetic acid (EDTA)‐grafted MOF‐808 is proposed to serve as a multifunctional ion‐selective separator coating, in which EDTA molecules play a targeted ion sifter role in restricting active‐ion crosstalk. Judicious characterizations and theoretical calculations reveal that the separator coating effectively captures the TM‐ions in the electrolyte and thus ensures stable Li deposition without dendrites. As a result, the 4.5 V NCM622//Li cell with the ion‐selective separator achieves a high‐capacity retention over 1000 cycles with a high Coulombic efficiency of 99.68%, and its cycling stability at 55 °C is also upgraded. This crosstalk‐taming strategy offers fresh insight into constructing long‐life HV‐LMBs.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Taming Active‐Ion Crosstalk by Targeted Ion Sifter Toward High‐Voltage Lithium Metal Batteries

Feng,

Zhong,

Zhang

et al. 2023

Advanced Energy Materials

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“…In the past ten years, researchers have employed a variety of advanced spatial-, time-, and energy-resolved characterization tools, in combination with theoretical simulations, to characterize the SEI composition and structure, with the aim of updating the knowledge of SEI chemistry. − For example, with the successful application of cryogenic transmission electron microscopy (cryo-EM), a number of literatures reported that the SEI exhibits a so-called plum pudding model (Figure c), in which an amorphous organic polymer matrix (termed “pudding”) was embedded with inorganic crystalline (known as “plums”). , Additionally, our group proposed an ultrasmooth ultrathin SEI for Li metal, which has proven to bear alternating organic–inorganic multilayered structure by employing atomic force microscope (AFM)-based indentation technique (Figure d). , Despite the variations in the detailed structure, the latest understanding of SEI remains fundamentally consistent with classical mosaic and layered models. Essentially, a precise knowledge regarding the SEI composition and structure as well as an accurate and comprehensive understanding of the formation and evolution mechanism and roles of the SEI in anode processes is still lacking.…”

Section: Introductionmentioning

confidence: 99%

Nanostructure-Based Plasmon-Enhanced Raman Spectroscopic Strategies for Characterization of the Solid–Electrolyte Interphase: Opportunities and Challenges

Tang

et al. 2023

J. Phys. Chem. C

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The physicochemical properties of the solid−electrolyte interphase (SEI) at anodes of lithium-based batteries are crucial for achieving the highest performance, and therefore, accurate characterizations are necessary to reveal the molecular structure and chemical properties of SEI. Nanostructure-based plasmonenhanced Raman spectroscopy (PERS) techniques rely on localized surface plasmonic enhancement mechanism and have offered significant opportunities, albeit with challenges, for nondestructive and real-time studies of SEI over the past two decades. In this Perspective, we highlight the recent progress in PERS, including surface-enhanced Raman spectroscopy (SERS), tip-enhanced Raman spectroscopy (TERS), and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) as a class of highly sensitive chemical fingerprint techniques for investigating the structure and chemistry of SEI. We also discuss the advantages and limitations of PERS for characterizing SEI and related interfacial processes. Lastly, we provide possible directions on how PERS can be further effectively leveraged to advance the characterization of interfaces and interphases of Li-based batteries, which could also be challenges for physical chemistry and energy chemistry.

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“…Advanced solid polymer electrolytes (SPEs) exhibit great potential for solid-state lithium metal batteries due to their high energy density and long lifespan. − Typically, poly(ethylene oxide) (PEO) and analogous copolymers have been extensively studied during the past several decades. − The critical challenges faced in these polymer electrolytes are to achieve high ionic conductivity (>10 –3 S cm –1 ) and electrochemical stability. Specific framework engineering, matrix modification, and topological polymers have been applied to overcome these obstacles.…”

Section: Introductionmentioning

confidence: 99%

Ion–Dipole-Interaction-Induced Encapsulation of Free Residual Solvent for Long-Cycle Solid-State Lithium Metal Batteries

Li,

An,

Song

et al. 2023

J. Am. Chem. Soc.

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Owing to high ionic conductivity and mechanical strength, poly(vinylidene fluoride) (PVDF) electrolytes have attracted increasing attention for solid-state lithium batteries, but highly reactive residual solvents severely plague cycling stability. Herein, we report a free-solvent-capturing strategy triggered by reinforced ion–dipole interactions between Li+ and residual solvent molecules. Lithium difluoro(oxalato)borate (LiDFOB) salt additive with electron-withdrawing capability serves as a redistributor of the Li+ electropositive state, which offers more binding sites for residual solvents. Benefiting from the modified coordination environment, the kinetically stable anion-derived interphases are preferentially formed, effectively mitigating the interfacial side reactions between the electrodes and electrolytes. As a result, the assembled solid-state battery shows a lifetime of over 2000 cycles with an average Coulombic efficiency of 99.9% and capacity retention of 80%. Our discovery sheds fresh light on the targeted regulation of the reactive residual solvent to extend the cycle life of solid-state batteries.

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Unravelling the convoluted and dynamic interphasial mechanisms on Li metal anodes

Cited by 47 publications

References 31 publications

Taming Active‐Ion Crosstalk by Targeted Ion Sifter Toward High‐Voltage Lithium Metal Batteries

Taming Active‐Ion Crosstalk by Targeted Ion Sifter Toward High‐Voltage Lithium Metal Batteries

Nanostructure-Based Plasmon-Enhanced Raman Spectroscopic Strategies for Characterization of the Solid–Electrolyte Interphase: Opportunities and Challenges

Ion–Dipole-Interaction-Induced Encapsulation of Free Residual Solvent for Long-Cycle Solid-State Lithium Metal Batteries

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