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Replacing conventional battery electrolyte additives with dioxolone derivatives for high-energy-density lithium-ion batteries.

ABSTRACT: Solid electrolyte interphases generated using electrolyte additives are key for anode-electrolyte interactions and for enhancing the lithium-ion battery lifespan. Classical solid electrolyte interphase additives, such as vinylene carbonate and fluoroethylene carbonate, have limited potential for simultaneously achieving a long lifespan and fast chargeability in high-energy-density lithium-ion batteries (LIBs). Here we report a next-generation synthetic additive approach that allows to form a highly stable electrode-electrolyte interface architecture from fluorinated and silylated electrolyte additives; it endures the lithiation-induced volume expansion of Si-embedded anodes and provides ion channels for facile Li-ion transport while protecting the Ni-rich LiNi_0.8Co_0.1Mn_0.1O₂ cathodes. The retrosynthetically designed solid electrolyte interphase-forming additives, 5-methyl-4-((trifluoromethoxy)methyl)-1,3-dioxol-2-one and 5-methyl-4-((trimethylsilyloxy)methyl)-1,3-dioxol-2-one, provide spatial flexibility to the vinylene carbonate-derived solid electrolyte interphase via polymeric propagation with the vinyl group of vinylene carbonate. The interface architecture from the synthesized vinylene carbonate-type additive enables high-energy-density LIBs with 81.5% capacity retention after 400 cycles at 1?C and fast charging capability (1.9% capacity fading after 100 cycles at 3?C).

SUBMITTER: Park S

PROVIDER: S-EPMC7864909 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Replacing conventional battery electrolyte additives with dioxolone derivatives for high-energy-density lithium-ion batteries.

Park Sewon S Jeong Seo Yeong SY Lee Tae Kyung TK Park Min Woo MW Lim Hyeong Yong HY Sung Jaekyung J Cho Jaephil J Kwak Sang Kyu SK Hong Sung You SY Choi Nam-Soon NS

Nature communications 20210205 1

Solid electrolyte interphases generated using electrolyte additives are key for anode-electrolyte interactions and for enhancing the lithium-ion battery lifespan. Classical solid electrolyte interphase additives, such as vinylene carbonate and fluoroethylene carbonate, have limited potential for simultaneously achieving a long lifespan and fast chargeability in high-energy-density lithium-ion batteries (LIBs). Here we report a next-generation synthetic additive approach that allows to form a hig ...[more]

PMID: 33547320

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Project description:The formation of a solid electrolyte interphase (SEI) between the anode surface and the electrolyte of lithium-ion batteries (LIBs) has been considered to be the most important yet the least understood issue of LIBs. To further our understanding in this regard, the density functional theory (DFT) B3PW91/6-311++G(3df,3pd) together with the implicit solvent model and the transition state theory were used for the first time to comprehensively explore the electroreduction mechanism of a novel additive, 4-chloromethyl-1,3,2-dioxathiolane-2-oxide (CMDO), and a few other solvents and additives, such as ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), fluoroethylene carbonate (FEC), and even ethylene sulfite (ES), for comparison. The one-electron reduction potential of Li+-coordinated compounds Li+(X) for forming decomposition precursors [c-Li+(X˙-)] decreases in the following sequence: CMDO (1.9-2.2 V vs. Li+/Li) ∼ ES(1.9 V) > FEC (0.7 V) > EC (0.47 V) > PC (0.45 V) > DMC (0.38 V); this implies that CMDO is reduced prior to other solvents or additives in the mixture. Although the ring opening of [c-Li+(CMDO˙-)] is the least kinetically favorable, as reflected by the highest energy barrier (E a), i.e., CMDO (18.8-22.9 kcal mol-1) ∼ ES (23.4) > FEC (16.2) > PC (12.5) > EC (11.2) > DMC (8.0), CMDO still shows the highest overall reaction rate constant (∼1053 s-1) for forming an open ring radical [o-Li+(CMDO˙)-]. In addition, the termination reaction of [o-Li+(CMDO˙)-] for forming LiCl is thermodynamically more favorable than that of Li2SO3 or organic disulfite (LiSO3)2-R, which supports the experimental observation that the halogen-containing LiF or LiCl additives are predominant over all other halogen-containing species in the SEI layer. Moreover, the hybrid model by including the second solvation shell of Li+ via a supercluster [(CMDO)Li+(PC)2](PC)9 and the implicit solvent model (SMD) can result in a reduction potential (∼1.7 V) that is in excellent agreement with the experimental reduction peak.

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Replacing conventional battery electrolyte additives with dioxolone derivatives for high-energy-density lithium-ion batteries.

Publications

Replacing conventional battery electrolyte additives with dioxolone derivatives for high-energy-density lithium-ion batteries.

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