Inorganic Filler Enhanced Formation of Stable Inorganic‐Rich Solid Electrolyte Interphase for High Performance Lithium Metal Batteries

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Abstract

Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO ₂not only accelerates Li ⁺transport but also regulates Li ⁺solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF‐rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE‐based Li||Cu half‐cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm ⁻²and 3 mAh cm ⁻², respectively. In addition, Li||LiFePO ₄full‐cells with a LM anode of limited Li supply of 4 mAh cm ⁻²achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g ⁻¹). Especially, when further applied in anode‐free LMBs, the carbon cloth||LiFePO ₄full‐cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C.

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Towards practical lithium-metal anodes

Xin Zhang, Yongan Yang, Zhen Zhen Zhou (2020)

Lithium ion batteries cannot meet the ever increasing demands of human society. Thus batteries with Li-metal anodes are eyed to revive. Here we summarize the recent progress in developing practical Li-metal anodes for various Li-based batteries. Lithium-ion batteries have had a tremendous impact on several sectors of our society; however, the intrinsic limitations of Li-ion chemistry limits their ability to meet the increasing demands of developing more advanced portable electronics, electric vehicles, and grid-scale energy storage systems. Therefore, battery chemistries beyond Li ions are being intensively investigated and need urgent breakthroughs toward commercial applications, wherein the use of metallic Li is one of the most intuitive choices. Despite several decades of oblivion due to safety concerns regarding the growth of Li dendrites, Li-metal anodes are now poised to be revived because of the advances in investigative tools and globally invested efforts. In this review, we first summarize the existing issues with regard to Li anodes and their underlying reasons and then highlight the recent progress made in the development of high-performance Li anodes. Finally, we propose the persisting challenges and opportunities toward the exploration of practical Li-metal anodes.

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High-voltage liquid electrolytes for Li batteries: progress and perspectives

Xiulin Fan, Chunsheng Wang (2021)

Recent advances, fundamental mechanisms and design strategies of high-voltage liquid electrolytes are comprehensively summarized in this review. Since the advent of the Li ion batteries (LIBs), the energy density has been tripled, mainly attributed to the increase of the electrode capacities. Now, the capacity of transition metal oxide cathodes is approaching the limit due to the stability limitation of the electrolytes. To further promote the energy density of LIBs, the most promising strategies are to enhance the cut-off voltage of the prevailing cathodes or explore novel high-capacity and high-voltage cathode materials, and also replacing the graphite anode with Si/Si–C or Li metal. However, the commercial ethylene carbonate (EC)-based electrolytes with relatively low anodic stability of ∼4.3 V vs. Li + /Li cannot sustain high-voltage cathodes. The bottleneck restricting the electrochemical performance in Li batteries has veered towards new electrolyte compositions catering for aggressive next-generation cathodes and Si/Si–C or Li metal anodes, since the oxidation-resistance of the electrolytes and the in situ formed cathode electrolyte interphase (CEI) layers at the high-voltage cathodes and solid electrolyte interphase (SEI) layers on anodes critically control the electrochemical performance of these high-voltage Li batteries. In this review, we present a comprehensive and in-depth overview on the recent advances, fundamental mechanisms, scientific challenges, and design strategies for the novel high-voltage electrolyte systems, especially focused on stability issues of the electrolytes, the compatibility and interactions between the electrolytes and the electrodes, and reaction mechanisms. Finally, novel insights, promising directions and potential solutions for high voltage electrolytes associated with effective SEI/CEI layers are proposed to motivate revolutionary next-generation high-voltage Li battery chemistries.