Diversity-oriented synthesis of polymer membranes with ion solvation cages

Baran, Miranda J.; Carrington, Mark E.; Sahu, Swagat; Baskin, Artem; Song, Junhua; Baird, Michael A.; Han, Kee Sung; Mueller, Karl T.; Teat, Simon J.; Meckler, Stephen M.; Fu, Chengyin; Prendergast, David; Helms, Brett A.

doi:10.1038/s41586-021-03377-7

Cited by 107 publications

(85 citation statements)

References 50 publications

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“…The most notable energy landscape for Cage E-Cage F Li + migration is estimated to be 0.7 eV (Figure 3i), which is comparable to that in sulfide or oxide-based solid electrolytes. [43,44] Because of strong ion-solvation, activated segmental motion, and improved diffusion kinetics, this theoretically supports the essential enhancement of ion-conduction in PHMO, which is concomitant with experimentally observed increases in ionic conductivity.…”

Section: Resultssupporting

confidence: 72%

An Ion‐Dipole‐Reinforced Polyether Electrolyte with Ion‐Solvation Cages Enabling High–Voltage‐Tolerant and Ion‐Conductive Solid‐State Lithium Metal Batteries

Zhang

Wang

et al. 2021

Adv Funct Materials

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Solid‐state electrolytes (SSEs) with sufficient ionic conduction, wide voltage window, flexible‐rigid interface, and ease of processibility are determinative to the development of energy‐dense solid‐state lithium metal batteries. Due to the low density and interfacial compatibility, polyether SSE has been studied for decades but remains handicapped by the inherently low ionic conductivity and insufficient voltage window. In this contribution, an ion‐dipole‐reinforced poly‐3‐hydroxymethyl‐3‐methyloxetane is demonstrated as a novel SSE and major substitution to conventional poly(ethylene oxide). By further polypropylene skeleton compositing, the composite solid electrolyte (PHMP) synergistically achieves high voltage tolerance (4.6 V), high ion‐conduction (25 °C, 1.26 × 10−4 S cm−1), and flexible‐rigid mechanical properties. Cryo‐transmission electron microscope has revealed a columnar Li deposition and LiF‐rich solid electrolyte interface, suggesting excellent dendrite suppression. According to density functional theory, the densely branched ether–oxygen groups play an important role as ion solvation cages, favoring strong Li+‐coordination and fast diffusion kinetics. More importantly, it restrains the proton‐induced decomposition and essentially enhances high‐voltage stability. As a result, PHMP contributes to an improved rate capability, significantly reduced interface impedance, and long‐term cycle stability of Li symmetrical batteries for over 1600 h. PHMP‐modified LiNi0.8Co0.1Mn0.1O2|Li batteries exhibit a high discharge capacity of 211.5 mAh g−1 and desirable cycle stability.

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Section: Resultssupporting

confidence: 72%

An Ion‐Dipole‐Reinforced Polyether Electrolyte with Ion‐Solvation Cages Enabling High–Voltage‐Tolerant and Ion‐Conductive Solid‐State Lithium Metal Batteries

Zhang

Wang

et al. 2021

Adv Funct Materials

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“…PIMs are widely used for gas adsorption and gas separation, 41 and recently also reported for many energy-related applications. 167,168…”

Section: Classification Of Popsmentioning

confidence: 99%

Emerging porous organic polymers for biomedical applications

et al. 2022

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“…There are a few recent studies that show that utilizing a liquid electrolyte in conjunction with a porous polymer structure can provide desirable transport properties and cycling performance in different lithium battery configurations [10][11][12][13][14]. Helms and colleagues reported a cation transference number of 0.72 for a nanoconfined polymer electrolyte based on a polymer of intrinsic microporosity (PIM) coated on lithium metal in 1 M LiTFSI and 0.2 M LiNO 3 (DOL-DME 1:1 v%) electrolyte [10].…”

Section: Introductionmentioning

confidence: 99%

Porous Polymer Gel Electrolytes Influence Lithium Transference Number and Cycling in Lithium-Ion Batteries

Boz

Ford

Salvadori

et al. 2021

Electronic Materials

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To improve the energy density of lithium-ion batteries, the development of advanced electrolytes with enhanced transport properties is highly important. Here, we show that by confining the conventional electrolyte (1 M LiPF6 in EC-DEC) in a microporous polymer network, the cation transference number increases to 0.79 while maintaining an ionic conductivity on the order of 10−3 S cm−1. By comparison, a non-porous, condensed polymer electrolyte of the same chemistry has a lower transference number and conductivity, of 0.65 and 7.6 × 10−4 S cm−1, respectively. Within Li-metal/LiFePO4 cells, the improved transport properties of the porous polymer electrolyte enable substantial performance enhancements compared to a commercial separator in terms of rate capability, capacity retention, active material utilization, and efficiency. These results highlight the importance of polymer electrolyte structure–performance property relationships and help guide the future engineering of better materials.

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Diversity-oriented synthesis of polymer membranes with ion solvation cages

Cited by 107 publications

References 50 publications

An Ion‐Dipole‐Reinforced Polyether Electrolyte with Ion‐Solvation Cages Enabling High–Voltage‐Tolerant and Ion‐Conductive Solid‐State Lithium Metal Batteries

An Ion‐Dipole‐Reinforced Polyether Electrolyte with Ion‐Solvation Cages Enabling High–Voltage‐Tolerant and Ion‐Conductive Solid‐State Lithium Metal Batteries

Emerging porous organic polymers for biomedical applications

Porous Polymer Gel Electrolytes Influence Lithium Transference Number and Cycling in Lithium-Ion Batteries

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