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Journal articles on the topic 'Polymer Electrolytes - Ion Dynamics'

Author: Grafiati

Published: 7 September 2023

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1

Mabuchi, Takuya, Koki Nakajima, and Takashi Tokumasu. "Molecular Dynamics Study of Ion Transport in Polymer Electrolytes of All-Solid-State Li-Ion Batteries." Micromachines 12, no. 9 (August 26, 2021): 1012. http://dx.doi.org/10.3390/mi12091012.

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Atomistic analysis of the ion transport in polymer electrolytes for all-solid-state Li-ion batteries was performed using molecular dynamics simulations to investigate the relationship between Li-ion transport and polymer morphology. Polyethylene oxide (PEO) and poly(diethylene oxide-alt-oxymethylene), P(2EO-MO), were used as the electrolyte materials, and the effects of salt concentrations and polymer types on the ion transport properties were explored. The size and number of LiTFSI clusters were found to increase with increasing salt concentrations, leading to a decrease in ion diffusivity at high salt concentrations. The Li-ion transport mechanisms were further analyzed by calculating the inter/intra-hopping rate and distance at various ion concentrations in PEO and P(2EO-MO) polymers. While the balance between the rate and distance of inter-hopping was comparable for both PEO and P(2EO-MO), the intra-hopping rate and distance were found to be higher in PEO than in P(2EO-MO), leading to a higher diffusivity in PEO. The results of this study provide insights into the correlation between the nanoscopic structures of ion solvation and the dynamics of Li-ion transport in polymer electrolytes.

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2

Kumar, Asheesh, Raghunandan Sharma, M. Suresh, Malay K. Das, and Kamal K. Kar. "Structural and ion transport properties of lithium triflate/poly(vinylidene fluoride-co-hexafluoropropylene)-based polymer electrolytes." Journal of Elastomers & Plastics 49, no. 6 (November 4, 2016): 513–26. http://dx.doi.org/10.1177/0095244316676512.

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Polymer electrolytes consisting of poly(vinylidene fluoride-co-hexafluoropropylene) in combination with lithium triflate (LiCF3SO3) salt of varying concentration have been prepared using the conventional solution casting technique in the argon atmosphere. Structural electrical characterizations of the synthesized electrolytes have been performed using various imaging and spectroscopic techniques. The DC conductivities determined by complex impedance plots reveal gradual increase with increase in salt concentration up to a particular limit and decrease subsequently. The maximum DC conductivity obtained at 300 K is 1.64 × 10−4 Scm−1 for the electrolyte with a polymer to salt weight ratio of 1:1.8. The temperature-dependent conductivity followed a mixed Arrhenius and Vogel–Tamman–Fulcher type behaviour for the polymer electrolytes. From the Summerfield master curve plot, the conductivity of the solid polymer electrolytes is found to depend not only on ion dynamics but also on the segmental mobility of the polymer chains.

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3

Yusof, S. Z., H. J. Woo, and A. K. Arof. "Ion dynamics in methylcellulose–LiBOB solid polymer electrolytes." Ionics 22, no. 11 (May 25, 2016): 2113–21. http://dx.doi.org/10.1007/s11581-016-1733-y.

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4

Garaga, Mounesha N., Sahana Bhattacharyya, and Steve G. Greenbaum. "Achieving Enhanced Mobility of Ions in Ionic Liquid-Based Gel Polymer Electrolytes By Incorporating Inorganic Nanofibers for Li-Ion Battery." ECS Meeting Abstracts MA2022-02, no. 2 (October 9, 2022): 160. http://dx.doi.org/10.1149/ma2022-022160mtgabs.

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Polymer electrolytes have received much attention in Li-ion battery research because of their unique properties, such as, high ionic conductivity, high mechanical strength including good electrode-electrolyte contact. A major research has been focused on improving the conductivity while retaining the mechanical stability of polymer electrolytes. In this context, ionic liquid-based gel polymer electrolytes are an excellent candidate. A detailed NMR investigation of PMMA-ILs gels electrolytes probing the structure and dynamics of ions was recently reported.[1] The presence of ILs in polymer matrix not only improves the conductivity but also enhances the self-healing capability. In another study, self-healing capability that reduces the dendrite formation at the interface has been discovered, for example, in PVDF-HFP-ILs electrolyte.[2] In this regard, this work reports the possible ways to enhance the ionic conductivity of such polymer electrolyte further by adding Al2O3 nanofibers. A series of PVDF-HFP-ILs with 1M LiTFSI in EMIMTFSI at different ratios of Al2O3nanofibers were prepared through solution cast technique. The dynamics of ions confined within polymer-Al2O3 matrix was explored through Impedence and PFG NMR spectroscopy. The amorphocity and the distribution of Al2O3 nanofibers are studied through XRD and SEM-EDX analyses. Lastly, the local structure of ions and their interaction with polymer and Al2O3 nanofibers were established through a detailed solid-state NMR analyses detecting 1H, 27Al, 13C, 19F, 7Li nuclei including 2D 13C{1H} HETCOR experiments. A reasonable enhancement in terms of ionic conductivity was observed with the addition of Al2O3 nanofibers, which improves the conducting pathways within the polymer network. [1] M. N. Garaga, N. Jayakody, C. C. Fraenza, B. Itin, and S. Greenbaum, Journal of Molecular Liquids 329, 115454 (2021). [2] T. Chen, W. Kong, Z. Zhang, L. Wang, Y. Hu, G. Zhu, R. Chen, L. Ma, W. Yan, Y. Wang, J. Liu, and Z. Jin, Nano Energy 54, 17 (2018).

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5

Peters, Brandon L., Zhou Yu, Paul C. Redfern, Larry A. Curtiss, and Lei Cheng. "Effects of Salt Aggregation in Perfluoroether Electrolytes." Journal of The Electrochemical Society 169, no. 2 (February 1, 2022): 020506. http://dx.doi.org/10.1149/1945-7111/ac4c7a.

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Electrolytes comprised of polymers mixed with salts have great potential for enabling the use of Li metal anodes in batteries for increased safety. Ionic conductivity is one of the key performance metrics of these polymer electrolytes and achieving high room-temperature conductivity remains a challenge to date. For a bottom-up design of the polymer electrolytes, we must first understand how the structure of polyelectrolytes on a molecular level determines their properties. Here, we use classical molecular dynamics to study the solvation structure and ion diffusion in electrolytes composed of a short-chain perfluoroether with LiFSI or LiTFSI salts. Density functional theory is also used to provide some insights into the structures and energies of the salt interactions with the perfluoroether. We observe the formation of aggregates of salts in the fluorinated systems even at low salt concentrations. The fluorine-fluorine attraction in the solvent is the governing factor for creating the salt aggregates. The aggregates’ size and lifetime change with concentration and anion. These simulations provide an insight into the structure and dynamics of perfluoroether based electrolytes that can be used to improve Li-ion batteries.

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6

Park, Habin, Anthony Engler, Nian Liu, and Paul Kohl. "Dynamic Anion Delocalization of Single-Ion Conducting Polymer Electrolyte for High-Performance of Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 227. http://dx.doi.org/10.1149/ma2022-023227mtgabs.

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Lithium metal batteries (LMBs) have been considered as next-generation energy storages due to their extremely high theoretical specific capacity (3860 mAh g-1). However, current LMBs, using conventional liquid electrolytes, still could not fulfill the demand of soaring expansion of energy era, such as electrical vehicles, because of their safety issues, originated by uncontrollable electrolytic side reaction on the lithium, resulting unstable solid-electrolyte interphase (SEI) and vicious lithium dendritic growth [1]. Also, carbonate-based liquid electrolytes have an intrinsic flammability, and the lithium dendrite, which short-circuits a cell, can lead to severe safety hazard with the unfavorable flammability of current liquid system when they are ignited. Therefore, solid-state electrolytes have been spotlighted recently for a pathway for safe, and high energy and power LMBs, due to their superior thermal stability and low vapor pressure, while maintaining suitable electrolytic performances. In this study, solid-state single-ion conducting polymer electrolytes (SICPEs), utilizing dynamic anion delocalization (DAD), realizing high ionic conductivity and dimensional stability for high-performance LMB, are studied. The SICPEs enable superior lithium transference number, resulting in highly reduced concentration gradient of lithium cation along the electrolyte to suppress the undesirable lithium dendritic growth. However, SICPEs have prominently lower ionic conductivity than dual-ion conducting polymer electrolyte (DICPEs), which is a critical issue to make a slower charge/discharge for SICPEs [2]. Although an approach utilizing gel polymer electrolyte (GPE), using a liquid solvent as a plasticizer, has been exploited to increase the ionic conductivity of SICPEs, GPEs have struggled with lower mechanical stability, compared to solid state, and still existing flammability issue with the plasticizer. The novel plasticizer, which is described here, can interact with bulky anionic polymer matrix, so that the negative charge can be dispersed onto the whole complex by DAD. Once the bulky complex is formed by DAD, the dissociation of lithium cation from anionic matrix can be easier with the decreased activation energy and higher ionic conduction. While increasing the ionic conductivity with DAD, the nature of polymeric plasticizer will highly suppress flammability. DAD allows the membrane endure more tensile strength due to the dynamic structural change in crosslinking state, so that the polymer electrolyte can tolerate dendritic growth of lithium by morphological change on an electrode surface. The obvious advantages of DAD-induced solid polymer electrolytes in this study for a high energy and power, and ultra-safe LMB can present a novel approach of polymer electrolyte design to the astronomical demand of energy storages. [1] F. Ahmed, I. Choi, M.M. Rahman, H. Jang, T. Ryu, S. Yoon, L. Jin, Y. Jin, W. Kim, ACS Appl. Mater. Interfaces 2019, 11, 34930-34938. [2] D.-M. Shin, J.E. Bachman, M.K. Taylor, J. Kamcev, J.G. Park, M.E. Ziebel, E. Velasquez, N.N. Jarenwattananon, G.K. Sethi, Y. Cui, J.R. Long, Adv. Mater. 2020, 32, 1905771.

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7

Dennis, John Ojur, Abdullahi Abbas Adam, M. K. M. Ali, Hassan Soleimani, Muhammad Fadhlullah Bin Abd Shukur, K. H. Ibnaouf, O. Aldaghri, et al. "Substantial Proton Ion Conduction in Methylcellulose/Pectin/Ammonium Chloride Based Solid Nanocomposite Polymer Electrolytes: Effect of ZnO Nanofiller." Membranes 12, no. 7 (July 13, 2022): 706. http://dx.doi.org/10.3390/membranes12070706.

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In this research, nanocomposite solid polymer electrolytes (NCSPEs) comprising methylcellulose/pectin (MC/PC) blend as host polymer, ammonium chloride (NH4Cl) as an ion source, and zinc oxide nanoparticles (ZnO NPs) as nanofillers were synthesized via a solution cast methodology. Techniques such as Fourier transform infrared (FTIR), electrical impedance spectroscopy (EIS), and linear sweep voltammetry (LSV) were employed to characterize the electrolyte. FTIR confirmed that the polymers, NH4Cl salt, and ZnO nanofiller interact with one another appreciably. EIS demonstrated the feasibility of achieving a conductivity of 3.13 × 10−4 Scm−1 for the optimum electrolyte at room temperature. Using the dielectric formalism technique, the dielectric properties, energy modulus, and relaxation time of NH4Cl in MC/PC/NH4Cl and MC/PC/NH4Cl/ZnO systems were determined. The contribution of chain dynamics and ion mobility was acknowledged by the presence of a peak in the imaginary portion of the modulus study. The LSV measurement yielded 4.55 V for the comparatively highest conductivity NCSPE.

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8

George, Sweta Mariam, Debalina Deb, Haijin Zhu, S. Sampath, and Aninda J. Bhattacharyya. "Spectroscopic investigations of solvent assisted Li-ion transport decoupled from polymer in a gel polymer electrolyte." Applied Physics Letters 121, no. 22 (November 28, 2022): 223903. http://dx.doi.org/10.1063/5.0112647.

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We present here a gel polymer electrolyte, where the Li+-ion transport is completely decoupled from the polymer host solvation and dynamics. A free-standing gel polymer electrolyte with a high volume content (nearly 60%) of xM LiTFSI in G4 (tetraglyme) ( x = 1–7; Li+:G4 = 0.2–1.5) liquid electrolyte confined inside the PAN (polyacrylonitrile)-PEGMEMA [poly (ethylene glycol) methyl ether methacrylate oligomer] based polymer matrix is synthesized using a one-pot free radical polymerization process. For LiTFSI concentrations, x = 1–7 (Li+:G4 = 0.2–1.5), Raman and vibrational spectroscopies reveal that like in the liquid electrolyte, the designed gel polymer electrolytes (GPEs) also show direct coordination of Li+-ions with the tetraglyme leading to the formation of [Li(G4)]+. Coupled with the spectroscopic studies, impedance and nuclear magnetic resonance investigations also show that the ion transport is independent of the polymer segmental motion and is governed by the solvated species {[Li(G4)]+}, very similar to the scenario in ionic liquids. As a result, the magnitude of ionic conductivity and activation energies of the gel polymer electrolyte are very similar to that of the liquid electrolyte. The Li+-ion transport number for the GPE varied from 0.44 ( x = 1) to 0.5 ( x = 7) with the maximum being 0.52 at x = 5.

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9

Caradant, Lea, Nina Verdier, Gabrielle Foran, David Lepage, Arnaud Prébé, David Aymé-Perrot, and Mickaël Dollé. "The Influence of Polar Functional Groups in Hot-Melt Extruded Polymer Blend Electrolytes for Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 210. http://dx.doi.org/10.1149/ma2022-012210mtgabs.

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Following the COP26 Summit in November 2021, more than hundred countries pledged to reach zero-emission by 2070 at the latest and the major car manufacturers committed to selling only electric vehicles by 2040. Currently, lithium-ion batteries (LIBs) are among the most widely used storage systems because of their high energy and power densities and long lifespan.1 The early LIBs are composed of intercalation electrodes, electronically isolated by an ion-conducting organic liquid electrolyte. However, the use of liquid electrolytes presents some disadvantages – especially in regard to consumer safety – related to short-circuits and potential leakages of the flammable liquid solvent. Moreover, in the case of lithium metal batteries, the combination of a liquid electrolyte and a high-capacity lithium metal anode leads to the uncontrolled deposition of lithium during the reduction, forming dendrites between the electrodes. A promising way to avoid this instability and improve battery safety is to replace the liquid electrolyte with an ion-conducting solid electrolyte.2 Among them, solid polymer electrolytes (SPEs) represent one of the most attractive alternatives due to their capacity to effectively conduct ions and higher mechanical resistance than their liquid counterparts.3 An important criterion for selecting polymers for use in SPEs is their ability to dissolve lithium salts through polar functional groups. Salt dissolution results in the replacement of ion-ion interactions in the lithium salt, with ion-dipole interactions in the polymer. The transport mechanisms of these ion-conducting materials differ from those of liquid electrolytes. Cation transport in polymer involves two steps which are considered to be dissociated or not, depending on the model chosen (Arrhenius or Vogel-Fulcher-Tammann, respectively). The application of one of these models provides interesting information on the ionic mobility dynamics in SPEs and, in particular, on the interplay between ionic jumps and polymer chain mobility. In the Arrhenius model, ionic jumps occur between coordinating sites, without taking into account the influence of segmental relaxation. Conversely, the VTF equation implies a strong relationship between these parameters. According to previous studies, higher segmental motions in the amorphous phase of polymers mainly provide ionic transport, which explains the limited ionic conductivity of SPEs at ambient temperature (less than 10-5 S/cm). Another major limitation of SPEs is primarily related to their dual role as electrolyte and binder in composite electrodes, which requires contradictory requirements to be met. Indeed, SPEs must have both sufficient flexibility to allow good interfacial contact between the electrode components and sufficient rigidity to limit short circuits. Polymer blending has emerged as an economic and effective technique to develop new SPEs which may simultaneously combine properties of each polymer and control the intrinsic properties of the resulting blend by adjusting the formulation.4 Moreover, polymer blends can be obtained by a solvent-free processing method, which reduce SPE toxicity and production time (no solvent evaporation). However, polymer blending makes both the salt dissociation processes and the ionic transport more difficult to understand as both polymers can dissolve lithium salts with their polar functional groups. Each polymer has different ionic transport properties depending on its architecture and thermal properties. Currently, no systematic survey comparing the ability of polymers with various functional groups to dissolve lithium salts in blends has thus far been conducted. In this presentation, we will discuss the salt dissociation ability of polar functional groups in various polymer blend SPEs. These groups are limited to those that are most commonly present in SPEs : ether, nitrile, carbonate, ester, alcohol and amide.5 The blends presented have been obtained by extrusion, which allows the effect of solvents on salt/polymer interactions to be neglected. In this work, coupled FTIR, EDX and 7Li NMR analyses allow the interactions between LiTFSI and the polymer blends to be determined with a good degree of certainty. Our original study combines experimental and theoretical approaches to determine effects of polymers’ lithium salt solvating ability on polymer blend electrolyte properties and represents an advancement in understanding and optimizing polymer selection for SPEs, used in lithium-ion batteries. References Xie, W., Liu, X., He, R., Li, Y., Gao, X., Li, X., Peng, Z., Feng, S., Feng, X. and Yang, S. Journal of Energy Storage 2020, 32, 101837. Chen, R., Qu, W., Guo, X., Li, L. and Wu, F. Materials Horizons 2016, 3, 487-516. Gray, F. M. Solid polymer electrolytes, VCH New Tork 1991. Caradant, L., Lepage, D., Nicolle, P., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2020, 4943-4951. Caradant, L., Verdier, N., Foran, G., Lepage, D., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2021. Figure 1

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10

Caradant, Lea, Nina Verdier, Gabrielle Foran, David Lepage, Arnaud Prébé, David Aymé-Perrot, and Mickaël Dollé. "The Influence of Polar Functional Groups in Melt-Blended Polymers Used As New Solid Electrolytes for Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2423. http://dx.doi.org/10.1149/ma2022-0272423mtgabs.

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Following the COP26 Summit in November 2021, more than hundred countries pledged to reach zero-emission by 2070 at the latest and the major car manufacturers committed to selling only electric vehicles by 2040. Currently, lithium-ion batteries (LIBs) are among the most widely used storage systems because of their high energy and power densities and long lifespan.1 The early LIBs are composed of intercalation electrodes, electronically isolated by an ion-conducting organic liquid electrolyte. However, the use of liquid electrolytes presents some disadvantages – especially in regard to consumer safety – related to short-circuits and potential leakages of the flammable liquid solvent. Moreover, in the case of lithium metal batteries, the combination of a liquid electrolyte and a high-capacity lithium metal anode leads to the uncontrolled deposition of lithium during the reduction, forming dendrites between the electrodes. A promising way to avoid this instability and improve battery safety is to replace the liquid electrolyte with an ion-conducting solid electrolyte.2 Among them, solid polymer electrolytes (SPEs) represent one of the most attractive alternatives due to their capacity to effectively conduct ions and higher mechanical resistance than their liquid counterparts.3 An important criterion for selecting polymers for use in SPEs is their ability to dissolve lithium salts through polar functional groups. Salt dissolution results in the replacement of ion-ion interactions in the lithium salt, with ion-dipole interactions in the polymer. The transport mechanisms of these ion-conducting materials differ from those of liquid electrolytes. Cation transport in polymer involves two steps which are considered to be dissociated or not, depending on the model chosen (Arrhenius or Vogel-Tamman-Fulcher, respectively). The application of one of these models provides interesting information on the ionic mobility dynamics in SPEs and, in particular, on the interplay between ionic jumps and polymer chain mobility. According to previous studies, higher segmental motions in the amorphous phase of polymers mainly provide ionic transport, which explains the limited ionic conductivity of SPEs at ambient temperature (less than 10-5 S/cm). Another major limitation of SPEs is primarily related to their dual role as electrolyte and binder in composite electrodes, which requires contradictory requirements to be met. Indeed, SPEs must have both sufficient flexibility to allow good interfacial contact between the electrode components and sufficient rigidity to limit short circuits. Polymer blending has emerged as an economic and effective technique to develop new SPEs which may simultaneously combine properties of each polymer and control the intrinsic properties of the resulting blend by adjusting the formulation.4 Moreover, polymer blends can be obtained by a solvent-free processing method, which reduce SPE toxicity and production time and cost. However, polymer blending makes both the salt dissociation processes and the ionic transport more difficult to understand as both polymers can dissolve lithium salts with their polar groups. Each polymer has different ionic transport properties depending on its architecture and thermal properties. Currently, no systematic survey comparing the ability of polymers with various functional groups to dissolve lithium salts in blends has thus far been conducted. In this presentation, we will discuss the salt dissociation ability of polar functional groups in various polymer blend SPEs. These groups are limited to those that are most commonly present in SPEs : ether, nitrile, carbonate, ester, alcohol and amide.5 The blends presented have been obtained by extrusion, which allows the effect of solvents on salt/polymer interactions to be neglected. Coupled FTIR, EDX and 7Li NMR analyses allow the interactions between LiTFSI and the polymer blends to be determined with a good degree of certainty. Our original study combines experimental and theoretical approaches to determine effects of polymers’ lithium salt solvating ability on blend electrolyte properties. Finally, this survey highlights an ideal polymer couple with the most promising and complementary properties, usable as SPE for LIBs. Indeed, this blend presents encouraging properties, compared to single-polymer SPEs, such as higher ionic conductivities over a wide temperature range, as well as improved mechanical and thermal stability properties and cycling performances. References Xie, W., Liu, X., He, R., Li, Y., Gao, X., Li, X., Peng, Z., Feng, S., Feng, X. and Yang, S. Journal of Energy Storage 2020, 32, 101837. Chen, R., Qu, W., Guo, X., Li, L. and Wu, F. Materials Horizons 2016, 3, 487-516. Gray, F. M. Solid polymer electrolytes, VCH New Tork 1991. Caradant, L., Lepage, D., Nicolle, P., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2020, 4943-4951. Caradant, L., Verdier, N., Foran, G., Lepage, D., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2021. Figure 1

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11

Rushing, Jeramie C., Anit Gurung, and Daniel G. Kuroda. "Relation between microscopic structure and macroscopic properties in polyacrylonitrile-based lithium-ion polymer gel electrolytes." Journal of Chemical Physics 158, no. 14 (April 14, 2023): 144705. http://dx.doi.org/10.1063/5.0135631.

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Polymer gel electrolytes (PGE) have seen a renewed interest in their development because they have high ionic conductivities but low electrochemical degradation and flammability. PGEs are formed by mixing a liquid lithium-ion electrolyte with a polymer at a sufficiently large concentration to form a gel. PGEs have been extensively studied, but the direct connection between their microscopic structure and macroscopic properties remains controversial. For example, it is still unknown whether the polymer in the PGE acts as an inert, stabilizing scaffold for the electrolyte or it interacts with the ionic components. Here, a PGE composed of a prototypical lithium-carbonate electrolyte and polyacrylonitrile (PAN) is pursued at both microscopic and macroscopic levels. Specifically, this study focused on describing the microscopic and macroscopic changes in the PGE at different polymer concentrations. The results indicated that the polymer-ion and polymer–polymer interactions are strongly dependent on the concentration of the polymer and the lithium salt. In particular, the polymer interacts with itself at very high PAN concentrations (10% weight) resulting in a viscous gel. However, the conductivity and dynamics of the electrolyte liquid components are significantly less affected by the addition of the polymer. The observations are explained in terms of the PGE structure, which transitions from a polymer solution to a gel, containing a polymer matrix and disperse electrolyte, at low and high PAN concentrations, respectively. The results highlight the critical role that the polymer concentration plays in determining both the macroscopic properties of the system and the molecular structure of the PGE.

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12

Nti, Frederick, George W. Greene, Haijin Zhu, Patrick C. Howlett, Maria Forsyth, and Xiaoen Wang. "Anion effects on the properties of OIPC/PVDF composites." Materials Advances 2, no. 5 (2021): 1683–94. http://dx.doi.org/10.1039/d0ma00992j.

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13

Weber, Ryan L., and Mahesh K. Mahanthappa. "Thiol–ene synthesis and characterization of lithium bis(malonato)borate single-ion conducting gel polymer electrolytes." Soft Matter 13, no. 41 (2017): 7633–43. http://dx.doi.org/10.1039/c7sm01738c.

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14

Bhandary, Rajesh, and Monika Schönhoff. "Polymer effect on lithium ion dynamics in gel polymer electrolytes: Cationic versus acrylate polymer." Electrochimica Acta 174 (August 2015): 753–61. http://dx.doi.org/10.1016/j.electacta.2015.05.145.

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15

Kim, Young C., Brian L. Chaloux, Debra R. Rolison, Michelle D. Johannes, and Megan B. Sassin. "Molecular dynamics study of hydroxide ion diffusion in polymer electrolytes." Electrochemistry Communications 140 (July 2022): 107334. http://dx.doi.org/10.1016/j.elecom.2022.107334.

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16

Ramya, C. S., and S. Selvasekarapandian. "Spectroscopic studies on ion dynamics of PVP–NH4SCN polymer electrolytes." Ionics 20, no. 12 (May 4, 2014): 1681–86. http://dx.doi.org/10.1007/s11581-014-1130-3.

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17

Brinkkötter, M., M. Gouverneur, P. J. Sebastião, F. Vaca Chávez, and M. Schönhoff. "Spin relaxation studies of Li+ ion dynamics in polymer gel electrolytes." Physical Chemistry Chemical Physics 19, no. 10 (2017): 7390–98. http://dx.doi.org/10.1039/c6cp08756f.

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18

Chavan, Kanchan, Pallab Barai, Hong-Keun Kim, and Venkat Srinivasan. "Decoding the Ceramics Influence in the Composite Electrolytes." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 494. http://dx.doi.org/10.1149/ma2022-024494mtgabs.

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As Lithium-Ion Batteries (LIBs) becomes an essential part of the everyday life, fireproof electrolytes have become an important component of the next generation battery design without compromising the performance of the battery. Composite electrolytes (CEs), consist of polymer electrolytes with highly conducting ceramic particles are promising candidates to substitute currently commercialized LIBs with liquid electrolytes. So far, experiments with CEs have discovered positive and negative effect on the overall conductivity of the CEs in the presence of ceramic particles.1–4 Therefore, exists the conflict weather the CEs are the solution to overcome the disadvantages of all-liquid and all-solid electrolytes. In this work, a 2-Dimensional CE with a uniform ceramic particle size distribution is studied via continuum modeling. we analyze the effect of interface between polymer and ceramic particle on the overall conductivity and transference number of the CEs to guide experimentalist to fabricate these interfaces carefully. It is concluded that the interplay between ohmic resistance and polymer conductivity at the polymer and ceramic particle interfaces can explain the conflicts observed in the literature. The Ohmic resistance at the interface is a critical parameter that determines whether ceramic particles enhance the overall conductivity or not. Finally, CEs does meet the criteria of the conductivity and transference number requirement in order to use in the EVs.5 References: (1) Cheng, S. H.-S.; He, K.-Q.; Liu, Y.; Zha, J.-W.; Kamruzzaman, M.; Ma, R. L.-W.; Dang, Z.-M.; Li, R. K. Y.; Chung, C. Y. Electrochemical Performance of All-Solid-State Lithium Batteries Using Inorganic Lithium Garnets Particulate Reinforced PEO/LiClO4 Electrolyte. Electrochimica Acta 2017, 253, 430–438. (2) Zagórski, J.; López del Amo, J. M.; Cordill, M. J.; Aguesse, F.; Buannic, L.; Llordés, A. Garnet–Polymer Composite Electrolytes: New Insights on Local Li-Ion Dynamics and Electrodeposition Stability with Li Metal Anodes. ACS Appl. Energy Mater. 2019, 2 (3), 1734–1746. (3) Bonilla, M. R.; García Daza, F. A.; Ranque, P.; Aguesse, F.; Carrasco, J.; Akhmatskaya, E. Unveiling Interfacial Li-Ion Dynamics in Li 7 La 3 Zr 2 O 12 /PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteries. ACS Appl. Mater. Interfaces 2021, 13 (26), 30653–30667. (4) Choi, J.-H.; Lee, C.-H.; Yu, J.-H.; Doh, C.-H.; Lee, S.-M. Enhancement of Ionic Conductivity of Composite Membranes for All-Solid-State Lithium Rechargeable Batteries Incorporating Tetragonal Li7La3Zr2O12 into a Polyethylene Oxide Matrix. J. Power Sources 2015, 274, 458–463. (5) Kim, H.-K.; Srinivasan, V. Status and Targets for Polymer-Based Solid-State Batteries for Electric Vehicle Applications. J. Electrochem. Soc. 2020, 167 (13), 130520.

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19

Li, Guan Min. "Mathematical Model of Transmission Mechanism from Multiphase Composite System." Advanced Materials Research 850-851 (December 2013): 300–303. http://dx.doi.org/10.4028/www.scientific.net/amr.850-851.300.

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As part of the weak electrolyte, Multiphase Composite System’s structure is more complex. So the conductive electrolyte ion transport has some difficulty to understanding the mechanism. And the present study has not yet reached a consensus, but through the ion conduction mechanism in-depth research on polymer electrolytes Preparation of important guiding significance. Current theories include ionic conductivity effective medium theory (EMT), MN law, WFL equation, NE equation, dynamic bonding penetration model.

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Chen, X. Chelsea, Robert L. Sacci, Naresh C. Osti, Madhusudan Tyagi, Beth L. Armstrong, Yangyang Wang, Max J. Palmer, and Nancy J. Dudney. "Correction: Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering." Molecular Systems Design & Engineering 4, no. 4 (2019): 983. http://dx.doi.org/10.1039/c9me90023c.

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Correction for ‘Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering’ by X. Chelsea Chen et al., Mol. Syst. Des. Eng., 2019, 4, 379–385.

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Lee, Youngju, and Peng Bai. "Overlimiting Currents and Sand’s Time Behaviors in Solid Polymer Electrolytes." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 485. http://dx.doi.org/10.1149/ma2022-024485mtgabs.

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Dendrite growth in solid polymer electrolytes has been frequently analyzed since it was the critical issue that limited its applications. For the liquid electrolyte systems, the dilute solution theory and the classic Nernst-Planck equation have been proven to be useful tools for analysis of ion transport dynamics and especially the dendrite initiation at Sand’s time. However, characterization of the Sand’s time in solid polymer electrolyte systems is challenging and also seldomly performed. From the experimental perspective, operando observations have been done, but the true local current density was different from the geometrical average current density since there was always heterogeneous current distribution for millimeter-scale electrolytes. From the theoretical perspective, the dendrite initiation time followed the trend predicted by Sand’s equation, but discrepancies were found such as dendrites observed at under-limiting currents or the order-of-magnitude extended Sand’s time compared to theoretical predictions. Here, we use transparent microcapillary cells for solid polymer electrolyte systems to overcome these challenges. These specialized cells allow direct operando optical observations, while the micron-scale cross-sectional area minimizes the discrepancy between true local and averaged geometrical current densities. Comparison between operando image and voltage response during constant current polarization shows that, unlike liquid electrolyte cases, the dendrite initiation for solid polymer electrolytes doesn’t always trigger a voltage spike. We also derived transport parameters from the measured Sand’s time, limiting current density, and conductivity and the cross-validated transport parameters were used to calculate theoretical Sand’s time that can be compared with the experimental values. Using the analytical solution from the Nernst-Planck equation and numerical calculations using Newman’s concentrated solution model and COMSOL Multiphysics, the predicted Sand’s time for the dilute and concentrated solution theory both matched closely with our experimental values. This work demonstrates that while the polarization process and the onset of lithium dendritic growths in solid polymer electrolytes can be still accurately predicted by the dilute solution theory, it may not always result in voltage responses similar to that of the liquid electrolyte cases. It’s also suggested that ensuring the homogenous distribution of lithium flux and avoiding the localized overlimiting current density is the key to realizing the dendrite-free polymer electrolytes.

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Aziz, B. Marif, Brza, Hamsan, and Kadir. "Employing of Trukhan Model to Estimate Ion Transport Parameters in PVA Based Solid Polymer Electrolyte." Polymers 11, no. 10 (October 16, 2019): 1694. http://dx.doi.org/10.3390/polym11101694.

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In the current paper, ion transport parameters in poly (vinyl alcohol) (PVA) based solid polymer electrolyte were examined using Trukhan model successfully. The desired amount of lithium trifluoromethanesulfonate (LiCF3SO3) was dissolved in PVA host polymer to synthesis of solid polymer electrolytes (SPEs). Ion transport parameters such as mobility (μ), diffusion coefficient (D), and charge carrier number density (n) are investigated in detail using impedance spectroscopy. The data results from impedance plots illustrated a decrement of bulk resistance with an increase in temperature. Using electrical equivalent circuits (EEC), electrical impedance plots (ZivsZr) are fitted at various temperatures. The results of impedance study demonstrated that the resistivity of the sample decreases with increasing temperature. The decrease of resistance or impedance with increasing temperature distinguished from Bode plots. The dielectric constant and dielectric loss values increased with an increase in temperature. The loss tangent peaks shifted to higher frequency region and the intensity increased with an increase in temperature. In this contribution, ion transport as a complicated subject in polymer physics is studied. The conductivity versus reciprocal of temperature was found to obey Arrhenius behavior type. The ion transport mechanism is discussed from the tanδ spectra. The ion transport parameters at ambient temperature are found to be 9 × 10−8 cm2/s, 0.8 × 1017 cm−3, and 3 × 10−6 cm2/Vs for D, n, andμ respectively. All these parameters have shown increasing as temperature increased. The electric modulus parameters are studied in an attempt to understand the relaxation dynamics and to clarify the relaxation process and ion dynamics relationship.

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Liu, Jie, Lifang Zhang, Yufeng Cao, Zhenkang Wang, Xinyao Xia, Jinqiu Zhou, Xiaowei Shen, Xi Zhou, Tao Qian, and Chenglin Yan. "Water-tolerant solid polymer electrolyte with high ion-conductivity for simplified battery manufacturing in air surroundings." Applied Physics Letters 121, no. 15 (October 10, 2022): 153905. http://dx.doi.org/10.1063/5.0106897.

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The humidity-sensitive electrolytes necessitate the stringent conditions of lithium battery manufacturing and, thus, increase the fabrication complexity and cost. We herein report a water-tolerant solid polymer electrolyte (WT-SPE) with high Li+ conductivity (2.08 × 10−4 S cm−1 at room temperature) and electrochemically stable window (up to 4.7 V vs Li/Li+), which utilizes moisture to initiate rapid polymerization and form dense structures to achieve a facile battery manufacturing in humid air without the need of a glovebox. Molecular dynamics simulations attribute this hydrophobic behavior to the hindered transfer of a water molecule in dense WT-SPE. A stable SEI layer composed of a polymeric framework and other organic/inorganic small molecular compounds contributes to the sustainable operation of batteries. As a result, the Li|WT-SPE|LiCoO2 cells manufactured in the air exhibit a high initial capacity of 192 mA h g−1 at 0.1C and an excellent capacity retention for 300 cycles at 1C. The great advantage significantly simplifies the battery assembly process in air environment and can also maintain good interfacial contact between an electrolyte and electrodes thanks to in situ initiated polymerization, which shows great superiority and promise in the alternatives of traditional liquid and polymer electrolytes for low-cost and facile fabrication of batteries in ambient atmosphere.

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Xue, Xiaoyuan, Long Wan, Wenwen Li, Xueling Tan, Xiaoyu Du, and Yongfen Tong. "A Self-Healing Gel Polymer Electrolyte, Based on a Macromolecule Cross-Linked Chitosan for Flexible Supercapacitors." Gels 9, no. 1 (December 23, 2022): 8. http://dx.doi.org/10.3390/gels9010008.

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Gel polymer electrolytes with a satisfied ionic conductivity have attracted interest in flexible energy storage technologies, such as supercapacitors and rechargeable batteries. However, the poor mechanical strength inhibits its widespread application. One of the most significant ways to avoid the drawbacks of the gel polymer electrolytes without compromising their ion transportation capabilities is to create a self−healing structure with the cross−linking segment. Herein, a new kind of macromolecule chemical cross−linked network ionic gel polymer electrolyte (MCIGPE) with superior electrochemical characteristics, a high flexibility, and an excellent self−healing ability were designed, based on chitosan and dibenzaldehyde−terminated poly (ethylene glycol) (PEGDA) via dynamic imine bonds. The ionic conductivity of the MCIGPE−65 can achieve 2.75 × 10−2 S cm−1. A symmetric all−solid−state supercapacitor employing carbon cloth as current collectors, activated a carbon film as electrodes, and MCIGPE−65 as a gel polymer electrolyte exhibits a high specific capacitance of 51.1 F g−1 at 1 A g−1, and the energy density of 7.1 Wh kg−1 at a power density of 500.2 W kg−1. This research proves the enormous potential of incorporating, environmentally and economically, chitosan into gel polymer electrolytes for supercapacitors.

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Ahmad, Shahzada, and S. A. Agnihotry. "Effect of nano γ-Al2O3 addition on ion dynamics in polymer electrolytes." Current Applied Physics 9, no. 1 (January 2009): 108–14. http://dx.doi.org/10.1016/j.cap.2007.12.003.

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Selter, Philipp, Stefanie Grote, and Gunther Brunklaus. "Synthesis and7Li Ion Dynamics in Polyarylene-Ethersulfone-Phenylene-Oxide-Based Polymer Electrolytes." Macromolecular Chemistry and Physics 217, no. 23 (October 10, 2016): 2584–94. http://dx.doi.org/10.1002/macp.201600211.

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Srivastava, Neelam, and Manindra Kumar. "Ion dynamics behavior in solid polymer electrolyte." Solid State Ionics 262 (September 2014): 806–10. http://dx.doi.org/10.1016/j.ssi.2013.10.026.

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Tiwari, Tuhina, Neelam Srivastava, and P. C. Srivastava. "Ion Dynamics Study of Potato Starch + Sodium Salts Electrolyte System." International Journal of Electrochemistry 2013 (2013): 1–8. http://dx.doi.org/10.1155/2013/670914.

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The effect of different anions, namely,SCN−,I−, andClO4−, on the electrical properties of starch-based polymer electrolytes has been studied. Anion size and conductivity are having an inverse trend indicating systems to be predominantly anionic conductor. Impact of anion size and multiplet forming tendency is reflected in number of charge carriers and mobility, respectively. Ion dynamics study reveals the presence of different mechanisms in different frequency ranges. Interestingly, superlinear power law (SLPL) is found to be present at <5 MHz frequency, which is further confirmed by dielectric data.

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Sadiq, Niyaz M., Shujahadeen B. Aziz, and Mohd F. Z. Kadir. "Development of Flexible Plasticized Ion Conducting Polymer Blend Electrolytes Based on Polyvinyl Alcohol (PVA): Chitosan (CS) with High Ion Transport Parameters Close to Gel Based Electrolytes." Gels 8, no. 3 (March 2, 2022): 153. http://dx.doi.org/10.3390/gels8030153.

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In the current study, flexible films of polyvinyl alcohol (PVA): chitosan (CS) solid polymer blend electrolytes (PBEs) with high ion transport property close enough to gel based electrolytes were prepared with the aid of casting methodology. Glycerol (GL) as a plasticizer and sodium bromide (NaBr) as an ionic source provider are added to PBEs. The flexible films have been examined for their structural and electrical properties. The GL content changed the brittle and solid behavior of the films to a soft manner. X-ray diffraction (XRD) and Fourier transform infrared (FTIR) methods were used to examine the structural behavior of the electrolyte films. X-ray diffraction investigation revealed that the crystalline character of PVA:CS:NaBr declined with increasing GL concentration. The FTIR investigation hypothesized the interaction between polymer mix salt systems and added plasticizer. Infrared (FTIR) band shifts and fluctuations in intensity have been found. The ion transport characteristics such as mobility, carrier density, and diffusion were successfully calculated using the experimental impedance data that had been fitted with EEC components and dielectric parameters. CS:PVA at ambient temperature has the highest ionic conductivity of 3.8 × 10 S/cm for 35 wt.% of NaBr loaded with 55 wt.% of GL. The high ionic conductivity and improved transport properties revealed the suitableness of the films for energy storage device applications. The dielectric constant and dielectric loss were higher at lower frequencies. The relaxation nature of the samples was investigated using loss tangent and electric modulus plots. The peak detected in the spectra of tanδ and M” plots and the distribution of data points are asymmetric besides the peak positions. The movements of ions are not free from the polymer chain dynamics due to viscoelastic relaxation being dominant. The distorted arcs in the Argand plot have confirmed the viscoelastic relaxation in all the prepared films.

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Mustapa, Siti Rosnah, Min Min Aung, and Marwah Rayung. "Physico-Chemical, Thermal, and Electrochemical Analysis of Solid Polymer Electrolyte from Vegetable Oil-Based Polyurethane." Polymers 13, no. 1 (December 30, 2020): 132. http://dx.doi.org/10.3390/polym13010132.

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In this paper, we report the preparation of bio-based polyurethane (PU) from renewable vegetable oil. The PU was synthesized through the reaction between jatropha oil-based polyol and isocyanate in a one-shot method. Then, lithium perchlorate (LiClO4) salt was added to the polyurethane system to form an electrolyte film via a solution casting technique. The solid polymer electrolyte was characterized through several techniques such as nuclear magnetic resonance (NMR), Fourier transforms infrared (FTIR), electrochemical studies, thermal studies by differential scanning calorimetry (DSC), and dynamic mechanical analysis (DMA). The NMR analysis confirmed that the polyurethane was successfully synthesized and the intermolecular reaction had occurred in the electrolytes system. The FTIR results show the shifting of the carbonyl group (C=O), ether and ester group (C–O–C), and amine functional groups (N–H) in PU–LiClO4 electrolytes compared to the blank polyurethane, which suggests that interaction occurred between the oxygen and nitrogen atom and the Li+ ion as they acted as electron donors in the electrolytes system. DSC analysis shows a decreasing trend in glass transition temperature, Tg and melting point, Tm of the polymer electrolyte as the salt content increases. Further, DMA analysis shows similar behavior in terms of Tg. The ionic conductivity increased with increasing salt content until the optimum value. The dielectric analysis reveals that the highest conducting electrolyte has the lowest relaxation time. The electrochemical behavior of the PU electrolytes is in line with the Tg result from the thermal analysis.

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Chattoraj, Joyjit, Marisa Knappe, and Andreas Heuer. "Dependence of Ion Dynamics on the Polymer Chain Length in Poly(ethylene oxide)-Based Polymer Electrolytes." Journal of Physical Chemistry B 119, no. 22 (May 22, 2015): 6786–91. http://dx.doi.org/10.1021/jp512734g.

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32

Vogel, M., and T. Torbrügge. "Ion and polymer dynamics in polymer electrolytes PPO-LiClO4. I. Insights from NMR line-shape analysis." Journal of Chemical Physics 125, no. 5 (August 7, 2006): 054905. http://dx.doi.org/10.1063/1.2217945.

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33

Chen, X. Chelsea, Robert L. Sacci, Naresh C. Osti, Madhusudan Tyagi, Yangyang Wang, Max J. Palmer, and Nancy J. Dudney. "Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering." Molecular Systems Design & Engineering 4, no. 2 (2019): 379–85. http://dx.doi.org/10.1039/c8me00113h.

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34

Huang, Yage, Xintong Mei, and Yunlong Guo. "Segmental and interfacial dynamics quantitatively determine ion transport in solid polymer composite electrolytes." Journal of Applied Polymer Science 139, no. 20 (January 8, 2022): 52143. http://dx.doi.org/10.1002/app.52143.

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35

Bharati, Devesh Chandra, Horesh Kumar, and A. L. Saroj. "Chitosan-PEG-NaI based bio-polymer electrolytes: structural, thermal and ion dynamics studies." Materials Research Express 6, no. 12 (January 22, 2020): 125360. http://dx.doi.org/10.1088/2053-1591/ab66a3.

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36

Aziz, Shujahadeen B., Elham M. A. Dannoun, Mohamad A. Brza, Niyaz M. Sadiq, Muaffaq M. Nofal, Wrya O. Karim, Sameerahl I. Al-Saeedi, and Mohd F. Z. Kadir. "An Investigation into the PVA:MC:NH4Cl-Based Proton-Conducting Polymer-Blend Electrolytes for Electrochemical Double Layer Capacitor (EDLC) Device Application: The FTIR, Circuit Design and Electrochemical Studies." Molecules 27, no. 3 (February 2, 2022): 1011. http://dx.doi.org/10.3390/molecules27031011.

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In this report, the preparation of solid polymer electrolytes (SPEs) is performed from polyvinyl alcohol, methyl cellulose (PVA-MC), and ammonium chloride (NH4Cl) using solution casting methodology for its use in electrical double layer capacitors (EDLCs). The characterizations of the prepared electrolyte are conducted using a variety of techniques, including Fourier transform infrared spectroscopy (FTIR), electrical impedance spectroscopy (EIS), cyclic voltammetry (CV), and linear sweep voltammetry (LSV). The interaction between the polymers and NH4Cl salt are assured via FTIR. EIS confirms the possibility of obtaining a reasonably high conductance of the electrolyte of 1.99 × 10−3 S/cm at room temperature. The dielectric response technique is applied to determine the extent of the ion dissociation of the NH4Cl in the PVA-MC-NH4Cl systems. The appearance of a peak in the imaginary part of the modulus study recognizes the contribution of chain dynamics and ion mobility. Transference number measurement (TNM) is specified and is found to be (tion) = 0.933 for the uppermost conducting sample. This verifies that ions are the predominant charge carriers. From the LSV study, 1.4 V are recorded for the relatively high-conducting sample. The CV curve response is far from the rectangular shape. The maximum specific capacitance of 20.6 F/g is recorded at 10 mV/s.

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Vogel, M., and T. Torbrügge. "Ion and polymer dynamics in polymer electrolytes PPO–LiClO4.II. H2 and Li7 NMR stimulated-echo experiments." Journal of Chemical Physics 125, no. 16 (October 28, 2006): 164910. http://dx.doi.org/10.1063/1.2358990.

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38

Nicotera, Isabella, Ernestino Lufrano, Cataldo Simari, Apostolos Enotiadis, Sergio Brutti, Maryam Nojabaee, and Brigitta Sievert. "Nanoscale Ionic Materials for Nafion Based Nanocomposites Membranes As Single Lithium-Ion Conducting Polymer Electrolytes for Lithium Sulfur Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 229. http://dx.doi.org/10.1149/ma2022-012229mtgabs.

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Currently, rechargeable batteries with the lithium–sulfur (Li–S) chemistry has attracted great interest as one of the most promising candidates for next generation electrochemical energy storage systems. Research into these high energy density devices is critical to the development of thinner, lighter, and lower cost battery systems. One of the biggest obstacles for practical applications of Li-S batteries is caused by the soluble nature of the highly ordered lithium polysulfides (Li2Sn) in the organic electrolytes and induce a so-called “shuttle eﬀect”. A solid-state electrolyte (SPEs) could be a valid alternative in terms of reducing the polysulﬁdes dissolution and shuttle, as well as to protect the lithium metal anode and to minimize dendrite formation, which is beneﬁcial for improving the safety and cycle life of Li−S batteries. SPEs are typically dual-ion conductor systems both cations and anions are mobile and cause a concentration polarization leading to poor performances of batteries. Recently, single lithium-ion conducting solid polymer electrolytes (SLIC-SPEs) have been proposed for polymer electrolytes, where anions are covalently bonded to the polymer, inorganic backbone, or immobilized by anion acceptors and only the Li+ cation will contribute to a permanent flow of charge. They have advantages over conventional dual-ion conducting SPEs such as unity transference number, absence of harmful effect of anion polarization, extremely low rate of Li dendrite growth and immobilization of the lithium polysulfides in the lithium-sulfur (Li-S) batteries. Polymer electrolytes based on ionomers (e.g., Naﬁon) with easily ionizable groups (e.g., sulfonic groups covalently bonded to the polymer side-chains, −CF2SO3 −) are promising thanks to the high concentration of weakly coordinating anions (counterions). In this work, lithiated Naﬁon and Naﬁon-nanocomposites membranes based on Nanoscale Ionic Materials (NIMs) were synthesized, and their ionic conductivity and lithium transference number were investigated in common nonaqueous organic solvents (EC/PC and Glymes). A thorough and systematic study of the lithium-ion transport was conducted by p 1H and 7Li pulsed ﬁeld gradient (PFG) NMR spectroscopy and electrochemical impedance spectroscopy (EIS), while the mechanical properties of the film electrolytes have been tested by dynamic mechanical analysis (DMA) in a wide temperature range. The electrochemical studies have been conducted both in Li/Li symmetric cell and in secondary Li-S cells. The preliminary results are very interesting, showing ionic conductivities of the order of 5 × 10-4 S/ cm at 25°C satisfactory properties in terms of stability window and stability of the lithium stripping. The lithium transport number is very close to unity thus confirming the complete immobilization of the negative charge carriers.

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39

Zhang, Lei, Haiqi Gao, Lixiang Guan, Yuchao Li, and Qian Wang. "Polyzwitterion–SiO2 Double-Network Polymer Electrolyte with High Strength and High Ionic Conductivity." Polymers 15, no. 2 (January 16, 2023): 466. http://dx.doi.org/10.3390/polym15020466.

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The key to developing high-performance polymer electrolytes (PEs) is to achieve their high strength and high ionic conductivity, but this is still challenging. Herein, we designed a new double-network PE based on the nonhydrolytic sol–gel reaction of tetraethyl orthosilicate and in situ polymerization of zwitterions. The as-prepared PE possesses high strength (0.75 Mpa) and high stretchability (560%) due to the efficient dissipation energy of the inorganic network and elastic characteristics of the polymer network. In addition, the highest ionic conductivity of the PE reaches 0.44 mS cm−1 at 30 °C owning to the construction of dynamic ion channels between the polyzwitterion segments and between the polyzwitterion segments and ionic liquids. Furthermore, the inorganic network can act as Lewis acid to adsorb trace impurities, resulting in a prepared electrolyte with a high electrochemical window over 5 V. The excellent interface compatibility of the as-prepared PE with a Li metal electrode is also confirmed. Our work provides new insights into the design and preparation of high-performance polymer-based electrolytes for solid-state energy storage devices.

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Lee, Sung-Il, Martina Schömer, Huagen Peng, Kirt A. Page, Daniel Wilms, Holger Frey, Christopher L. Soles, and Do Y. Yoon. "Correlations between Ion Conductivity and Polymer Dynamics in Hyperbranched Poly(ethylene oxide) Electrolytes for Lithium-Ion Batteries." Chemistry of Materials 23, no. 11 (June 14, 2011): 2685–88. http://dx.doi.org/10.1021/cm103696g.

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41

Harrison, Jeffrey S., Dean A. Waldow, Phillip A. Cox, Rajiv Giridharagopal, Marisa Adams, Victoria Richmond, Sevryn Modahl, Megan Longstaff, Rodion Zhuravlev, and David S. Ginger. "Noncontact Imaging of Ion Dynamics in Polymer Electrolytes with Time-Resolved Electrostatic Force Microscopy." ACS Nano 13, no. 1 (December 19, 2018): 536–43. http://dx.doi.org/10.1021/acsnano.8b07254.

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42

Becher, Manuel, Simon Becker, Lukas Hecht, and Michael Vogel. "From Local to Diffusive Dynamics in Polymer Electrolytes: NMR Studies on Coupling of Polymer and Ion Dynamics across Length and Time Scales." Macromolecules 52, no. 23 (November 15, 2019): 9128–39. http://dx.doi.org/10.1021/acs.macromol.9b01400.

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43

Borah, Sandeepan, Jayanta K. Sarmah, and M. Deka. "Understanding uptake kinetics and ion dynamics in microporous polymer gel electrolytes reinforced with SiO2 nanofibers." Materials Science and Engineering: B 273 (November 2021): 115419. http://dx.doi.org/10.1016/j.mseb.2021.115419.

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44

Brinkkötter, Marc, Elena I. Lozinskaya, Denis O. Ponkratov, Yakov Vygodskii, Daniel F. Schmidt, Alexander S. Shaplov, and Monika Schönhoff. "Influence of Cationic Poly(ionic liquid) Architecture on the Ion Dynamics in Polymer Gel Electrolytes." Journal of Physical Chemistry C 123, no. 21 (May 8, 2019): 13225–35. http://dx.doi.org/10.1021/acs.jpcc.9b03089.

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45

Dürr, O., W. Dieterich, and A. Nitzan. "Coupled ion and network dynamics in polymer electrolytes: Monte Carlo study of a lattice model." Journal of Chemical Physics 121, no. 24 (2004): 12732. http://dx.doi.org/10.1063/1.1825371.

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46

Simari, Cataldo, Ernestino Lufrano, Luigi Coppola, and Isabella Nicotera. "Composite Gel Polymer Electrolytes Based on Organo-Modified Nanoclays: Investigation on Lithium-Ion Transport and Mechanical Properties." Membranes 8, no. 3 (August 24, 2018): 69. http://dx.doi.org/10.3390/membranes8030069.

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Composite gel polymer electrolytes (GPEs) based on organo-modified montmorillonite clays have been prepared and investigated. The organo-clay was prepared by intercalation of CTAB molecules in the interlamellar space of sodium smectite clay (SWy) through a cation-exchange reaction. This was used as nanoadditive in polyacrylonitrile/polyethylene-oxide blend polymer, lithium trifluoromethanesulphonate (LiTr) as salt and a mixture of ethylene carbonate/propylene carbonate as plasticizer. GPEs were widely characterized by DSC, SEM, and DMA, while the ion transport properties were investigated by AC impedance spectroscopy and multinuclear NMR spectroscopy. In particular, 7Li and 19F self-diffusion coefficients were measured by the pulse field gradient (PFG) method, and the spin-lattice relaxation times (T1) by the inversion recovery sequence. A complete description of the ions dynamics in so complex systems was achieved, as well as the ion transport number and ionicity index were estimated, proving that the smectite clay surfaces are able to “solvatate” both lithium and triflate ions and to create a preferential pathway for ion conduction.

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Hosseinioun, Ava, Pinchas Nürnberg, Monika Schönhoff, Diddo Diddens, and Elie Paillard. "Improved lithium ion dynamics in crosslinked PMMA gel polymer electrolyte." RSC Advances 9, no. 47 (2019): 27574–82. http://dx.doi.org/10.1039/c9ra05917b.

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Ionic transport was investigated in a PMMA gel electrolyte by electrochemical, Raman, PFG-NMR, e-NMR spectroscopies and ab initio calculations. The presence of the PMMA matrix reduces anionic mobility and decorrelates cationic and anionic transport.

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48

Bergstrom, Helen K., Kara D. Fong, and Bryan D. McCloskey. "The Role of Ion-Correlation in Reducing the Lithium Transference Number in Lithium-Ion Polyelectrolyte Solutions." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 203. http://dx.doi.org/10.1149/ma2022-023203mtgabs.

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Non-aqueous polyelectrolyte solutions (PESs) have been suggested as a promising route to high conductivity, high transference number (t+) electrolytes.1–3 State-of-the-art liquid electrolytes suffer from low t+, meaning the majority of ionic conductivity results from motion of the anion rather than the electrochemically active Li+ ion. Increasing t+ requires decreasing the mobility of the anion, which is dictated by both the diffusion of the anion as well as its net charge. PESs are intuitively appealing because anchoring the anion to a polymer backbone slows down the motion of the electrochemically inactive anion while maintaining higher ion conductivity through improved ion dissociation and solvent-mediated Li+ transport. However, in polyelectrolyte systems, increasing molecular weight both decreases polymer diffusion and increases charge, which will act as competing effects for t+.Recent molecular dynamic simulations of PESs have highlighted the critical importance of correlated ion motion in these systems and have called into question oligomeric PESs as a feasible strategy to achieving high t+ and conductivity electrolytes4,5 In this work we discuss complete studies of transport properties in lithium-ion and lithium metal battery-relevant PESs- specifically lithium triflimide appended polystyrene (PS-LiTFSI) and polymethacrylate (PM-LiTFSI) dissolved in carbonate blends. All prior PES experimental work in the literature has relied on ideal solution assumptions for measuring transport properties. This work represents the first rigorous characterization of transport properties for a battery-relevant polyelectrolyte solution. Using electrophoretic NMR and electrochemical experiments, we characterized the transport properties, including the electrophoretic ion mobilities, conductivity, diffusion coefficients, and t+ of these model PESs. While previous studies that rely on ideal assumptions predict that PESs will have higher t+ than monomeric solutions, we demonstrate that below the entanglement limit, t+ decreases with increasing degree of polymerization. For higher degrees of polymerization, we directly observe Li+ move in the “wrong direction” in an electric field, evidence of a negative transference number due to correlated motion through ion clustering. Using calculated Onsager transport coefficients and insights from molecular dynamics modeling, we demonstrate that despite selectively slowing anion motion using polyanions, anion-anion correlation through the polymer backbone and cation-anion correlation through ion aggregates reduce the t+ in non-entangled PESs. References Diederichsen, K. M. et al. ACS Energy Lett. (2017). Diederichsen, K. M. et al. Macromolecules (2018). Dewing, B. L., et al. Chem. Mater. (2020). Fong, K. D. et al. ACS Cent. Sci. (2019). Fong, K. D., et al. Macromolecules (2020).

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Mongcopa, Katrina Irene S., Daniel A. Gribble, Whitney S. Loo, Madhusudan Tyagi, Scott A. Mullin, and Nitash P. Balsara. "Segmental Dynamics Measured by Quasi-Elastic Neutron Scattering and Ion Transport in Chemically Distinct Polymer Electrolytes." Macromolecules 53, no. 7 (March 31, 2020): 2406–11. http://dx.doi.org/10.1021/acs.macromol.0c00091.

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Bennington, Peter, Chuting Deng, Daniel Sharon, Michael A. Webb, Juan J. de Pablo, Paul F. Nealey, and Shrayesh N. Patel. "Role of solvation site segmental dynamics on ion transport in ethylene-oxide based side-chain polymer electrolytes." Journal of Materials Chemistry A 9, no. 15 (2021): 9937–51. http://dx.doi.org/10.1039/d1ta00899d.

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