Suppressing lithium dendrites within inorganic solid-state electrolytes

Lv, Qiang; Jiang, Yunpeng; Wang, Bo; Chen, Yujia; Jin, Fan; Wu, Bingxin; Ren, Huaizheng; Zhang, Nan; Xu, Ruoyu; Li, Yaohua; Zhang, Tianren; Zhou, Yu; Wang, Dianlong; Liu, Huan; Dou, S. X.

doi:10.1016/j.xcrp.2021.100706

Cited by 44 publications

(30 citation statements)

References 163 publications

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“…Among other major mechanisms, e.g., penetration through macroscopic defects such as voids or pores [ 68 ], dendrite growth in SSEs has been attributed to high local electronic conductivity, directly reducing Li

ions to metallic Li [ 7 , 69 , 70 ]. Suppression of Li(0) nucleation becomes even more crucial in the grain boundary region as these form networks that provide an often easily accessible route for further dendrite growth and penetration [ 7 , 71 ].…”

Section: Resultsmentioning

confidence: 99%

Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping

2022

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While great effort has been focused on bulk material design for high-performance All Solid-State Batteries (ASSBs), solid-solid interfaces, which typically extend over a nanometer regime, have been identified to severely impact cell performance. Major challenges are Li dendrite penetration along the grain boundary network of the Solid-State Electrolyte (SSE) and reductive decomposition at the electrolyte/electrode interface. A naturally forming nanoscale complexion encapsulating ceramic Li1+xAlxTi2−x(PO4)3 (LATP) SSE grains has been shown to serve as a thin protective layer against such degradation mechanisms. To further exploit this feature, we study the interfacial doping of divalent Mg2+ into LATP grain boundaries. Molecular Dynamics simulations for a realistic atomistic model of the grain boundary reveal Mg2+ to be an eligible dopant candidate as it rarely passes through the complexion and thus does not degrade the bulk electrolyte performance. Tuning the interphase stoichiometry promotes the suppression of reductive degradation mechanisms by lowering the Ti4+ content while simultaneously increasing the local Li+ conductivity. The Mg2+ doping investigated in this work identifies a promising route towards active interfacial engineering at the nanoscale from a computational perspective.

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Section: Resultsmentioning

confidence: 99%

Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping

2022

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“…Researchers hope to prevent the growth and penetration of lithium dendrites via inorganic solid electrolytes with high mechanical strength. With the development of characterization techniques, researchers have found that although the high mechanical strength of inorganic SSE could theoretically resist dendrite growth, Li dendrites still appear in the bulk phase of inorganic SSEs, eventually penetrating the SSE and causing short circuiting in the battery [ 26 ]. On the one hand, the crystal structure of inorganic SSE electrolytes promotes the growth of Li dendrites.…”

Section: Principles and Challenges Of Lithium–sulfur Batteriesmentioning

confidence: 99%

Solid-State Electrolytes for Lithium–Sulfur Batteries: Challenges, Progress, and Strategies

2022

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Lithium–sulfur batteries (LSBs) represent a promising next-generation energy storage system, with advantages such as high specific capacity (1675 mAh g−1), abundant resources, low price, and ecological friendliness. During the application of liquid electrolytes, the flammability of organic electrolytes, and the dissolution/shuttle of polysulfide seriously damage the safety and the cycle life of lithium–sulfur batteries. Replacing a liquid electrolyte with a solid one is a good solution, while the higher mechanical strength of solid-state electrolytes (SSEs) has an inhibitory effect on the growth of lithium dendrites. However, the lower ionic conductivity, poor interfacial contact, and relatively narrow electrochemical window of solid-state electrolytes limit the commercialization of solid-state lithium–sulfur batteries (SSLSBs). This review describes the research progress in LSBs and the challenges faced by SSEs, which are classified as polymer electrolytes, inorganic solid electrolytes, and composite electrolytes. The advantages, as well as the disadvantages of various types of electrolytes, the common coping strategies to improve performance, and future development trends, are systematically described.

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“…Due to the zero memory effect and long cycle life, lithium-(Li-) ion batteries (LIBs) composed of graphite anode and LiFePO 4 , LiCoO 2 (LCO), or LiNi x Mn y Co 1-x-y O 2 (NMC) cathodes play an irreplaceable role in almost every aspect of our life [1][2][3][4][5][6][7]. However, the energy density of LIBs can hardly exceed the upper limit of 300 Wh kg -1 [8,9]. By contrast, Li metal becomes the preferred anode for high-energy-density cells for its ultralow redox potential (-3.040 V versus the standard hydrogen electrode) and incomparable theoretical capacity (3862 mAh g -1 ) [6,10,11].…”

Section: Introductionmentioning

confidence: 99%

Electrolyte Engineering for High-Voltage Lithium Metal Batteries

et al. 2022

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High-voltage lithium metal batteries (HVLMBs) have been arguably regarded as the most prospective solution to ultrahigh-density energy storage devices beyond the reach of current technologies. Electrolyte, the only component inside the HVLMBs in contact with both aggressive cathode and Li anode, is expected to maintain stable electrode/electrolyte interfaces (EEIs) and facilitate reversible Li+ transference. Unfortunately, traditional electrolytes with narrow electrochemical windows fail to compromise the catalysis of high-voltage cathodes and infamous reactivity of the Li metal anode, which serves as a major contributor to detrimental electrochemical performance fading and thus impedes their practical applications. Developing stable electrolytes is vital for the further development of HVLMBs. However, optimization principles, design strategies, and future perspectives for the electrolytes of the HVLMBs have not been summarized in detail. This review first gives a systematical overview of recent progress in the improvement of traditional electrolytes and the design of novel electrolytes for the HVLMBs. Different strategies of conventional electrolyte modification, including high concentration electrolytes and CEI and SEI formation with additives, are covered. Novel electrolytes including fluorinated, ionic-liquid, sulfone, nitrile, and solid-state electrolytes are also outlined. In addition, theoretical studies and advanced characterization methods based on the electrolytes of the HVLMBs are probed to study the internal mechanism for ultrahigh stability at an extreme potential. It also foresees future research directions and perspectives for further development of electrolytes in the HVLMBs.

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Suppressing lithium dendrites within inorganic solid-state electrolytes

Cited by 44 publications

References 163 publications

Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping

Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping

Solid-State Electrolytes for Lithium–Sulfur Batteries: Challenges, Progress, and Strategies

Electrolyte Engineering for High-Voltage Lithium Metal Batteries

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