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Li, Z., Mindemark, J., Brandell, D. & Tominaga, Y. (2019). A concentrated poly(ethylene carbonate)/poly(trimethylene carbonate) blend electrolyte for all-solid-state Li battery. Polymer journal, 51(8), 753-760
Open this publication in new window or tab >>A concentrated poly(ethylene carbonate)/poly(trimethylene carbonate) blend electrolyte for all-solid-state Li battery
2019 (English)In: Polymer journal, ISSN 0032-3896, E-ISSN 1349-0540, Vol. 51, no 8, p. 753-760Article in journal (Refereed) Published
Abstract [en]

Electrochemical and ion-transport properties of polymer blend electrolytes comprising poly(ethylene carbonate) (PEC), poly (trimethylene carbonate) (PTMC) and lithium bis(fluorosulfonyl) imide (LiFSI) were studied in this work, and the electrolyte with the best blend composition was applied in all-solid-state Li batteries. The ionic conductivity of both PEC and PTMC single-polymer electrolytes increased with increasing Li salt concentration. All PEC and PTMC blend electrolytes show ionic conductivities on the order of 10(-5) S cm(-1) at 50 degrees C, and the ionic conductivities increase slightly with increasing PEC contents. The PEC6PTMC4-LiFSI 150 mol% electrolyte demonstrated better Li/electrolyte electrochemical and interfacial stability than that of PEC and PTMC single-polymer electrolytes and maintained a polarization as low as 5 mV for up to 200 h during Li metal plating and stripping. A Li vertical bar SPE vertical bar LFP cell with the PEC6PTMC4-LiFSI 150 mol% electrolyte exhibited reversible charge/discharge capacities close to 150 mAh g(-1) at 50 degrees C and a C/10 rate, which is 88% of the theoretical value (170 mAh g(-1)).

Place, publisher, year, edition, pages
NATURE PUBLISHING GROUP, 2019
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-392567 (URN)10.1038/s41428-019-0184-5 (DOI)000478790200005 ()
Funder
StandUp
Available from: 2019-09-10 Created: 2019-09-10 Last updated: 2019-09-10Bibliographically approved
Ebadi, M., Marchiori, C., Mindemark, J., Brandell, D. & Araujo, C. M. (2019). Assessing structure and stability of polymer/lithium-metal interfaces from first-principles calculations. Journal of Materials Chemistry A, 7(14), 8394-8404
Open this publication in new window or tab >>Assessing structure and stability of polymer/lithium-metal interfaces from first-principles calculations
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2019 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, no 14, p. 8394-8404Article in journal (Refereed) Published
Abstract [en]

Solid polymer electrolytes (SPEs) are promising candidates for Li metal battery applications, but the interface between these two categories of materials has so far been studied only to a limited degree. A better understanding of interfacial phenomena, primarily polymer degradation, is essential for improving battery performance. The aim of this study is to get insights into atomistic surface interaction and the early stages of solid electrolyte interphase formation between ionically conductive SPE host polymers and the Li metal electrode. A range of SPE candidates are studied, representative of major host material classes: polyethers, polyalcohols, polyesters, polycarbonates, polyamines and polynitriles. Density functional theory (DFT) calculations are carried out to study the stability and the electronic structure of such polymer/Li interfaces. The adsorption energies indicated a stronger adhesion to Li metal of polymers with ester/carbonate and nitrile functional groups. Together with a higher charge redistribution, a higher reactivity of these polymers is predicted as compared to the other electrolyte hosts. Products such as alkoxides and CO are obtained from the degradation of ester- and carbonate-based polymers by AIMD simulations, in agreement with experimental studies. Analogous to low-molecular-weight organic carbonates, decomposition pathways through C-carbonyl-O-ethereal and C-ethereal-O-ethereal bond cleavage can be assumed, with carbonate-containing fragments being thermodynamically favorable.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-382550 (URN)10.1039/c8ta12147h (DOI)000464414200040 ()
Funder
Swedish Energy Agency, 39036-1Swedish Research Council, 621-2014-5984EU, European Research Council, 771777Carl Tryggers foundation
Available from: 2019-05-10 Created: 2019-05-10 Last updated: 2019-08-05Bibliographically approved
Eriksson, T., Mindemark, J., Yue, M. & Brandell, D. (2019). Effects of nanoparticle addition to poly(epsilon-caprolactone) electrolytes: Crystallinity, conductivity and ambient temperature battery cycling. Electrochimica Acta, 300, 489-496
Open this publication in new window or tab >>Effects of nanoparticle addition to poly(epsilon-caprolactone) electrolytes: Crystallinity, conductivity and ambient temperature battery cycling
2019 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 300, p. 489-496Article in journal (Refereed) Published
Abstract [en]

It has previously been shown that nanoparticle additives can, in a simple way, significantly improve the ionic conductivity in solid polymer electrolyte systems with the semi-crystalline poly(ethylene oxide) (PEO) as a host material. It has been suggested that the improved ionic conductivity is a result of reduced degree of crystallinity and additional conductivity mechanisms occurring in the material. In this work, this principle is applied to another semi-crystalline polymer host: poly(epsilon-caprolactone) (PCL). This is a polymer with comparable properties (T-g, T-m, etc.) as PEO, and constitute a promising material for use in solid polymer electrolytes for lithium ion batteries. 15 wt% of the respective nanoparticles TiO2, Al2O3 and h-BN have been added to the PCL-LiTFSI solid polymer electrolyte in an attempt to increase the conductivity and achieve stable room temperature cyclability. The crystallinity, ionic conductivity and electrochemical properties were investigated by differential scanning calorimetry, electrochemical impedance spectroscopy and galvanostatic cycling of cells. The results showed that with an addition of 15 wt% Al2O3, the degree of crystallinity is reduced to 6-7% and the ionic conductivity increased to 6-7 x 10(-6) S cm(-1) at room temperature, allowing successful cycling of cells at 30 degrees C, while h-BN did not contribute to similar improvements. The effect of nanoparticles, however, differ significantly from previous observations in PEO systems, which could be explained by different surface-polymer interactions or the degree of ordering in the amorphous phases of the materials.

Place, publisher, year, edition, pages
PERGAMON-ELSEVIER SCIENCE LTD, 2019
Keywords
Li-battery, Solid polymer electrolyte, Polyester, Nanoparticle
National Category
Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:uu:diva-378621 (URN)10.1016/j.electacta.2019.01.117 (DOI)000458488200058 ()
Funder
EU, Horizon 2020, 685716The Swedish Foundation for International Cooperation in Research and Higher Education (STINT), CH2016-6753
Available from: 2019-03-11 Created: 2019-03-11 Last updated: 2019-03-11Bibliographically approved
Sångeland, C., Mogensen, R., Brandell, D. & Mindemark, J. (2019). Stable Cycling of Sodium Metal All-Solid-State Batteries with Polycarbonate-Based Polymer Electrolytes. ACS APPLIED POLYMER MATERIALS, 1(4), 825-832
Open this publication in new window or tab >>Stable Cycling of Sodium Metal All-Solid-State Batteries with Polycarbonate-Based Polymer Electrolytes
2019 (English)In: ACS APPLIED POLYMER MATERIALS, ISSN 2637-6105, Vol. 1, no 4, p. 825-832Article in journal (Refereed) Published
Abstract [en]

Solid polymer electrolytes based on high-molecular-weight poly(trimethylene carbonate) (PTMC) in combination with NaFSI salt were investigated for application in sodium batteries. The polycarbonate host material proved to be able to dissolve large amounts of salt, at least up to a carbonate:Na+ ratio of 1:1. Combined DSC, conductivity, and FTIR data indicated the formation of a percolating network of salt clusters along with the transition to a percolation-type ion transport mechanism at the highest salt concentrations. While the highest total ionic conductivities were seen at the highest salt concentrations (up to a remarkable 5 x 10(-5) S cm(-1) at 25 degrees C at a 1:1 carbonate:Na+ ratio), the most stable battery performance was seen at a more moderate salt loading of 5:1 carbonate:Na+, reaching >80 cycles at a stable capacity of similar to 90 mAh g(-1) at 60 degrees C in a sodium metal/Prussian blue cell. The results highlight the importance of the choice of salt and salt concentration on electrolyte performance as well as demonstrate the potential of utilizing polycarbonate-based electrolytes in sodium-based energy storage systems.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
Keywords
polymer electrolytes, polycarbonates, sodium, batteries, ionic conductivity
National Category
Polymer Chemistry Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-392889 (URN)10.1021/acsapm.9b00068 (DOI)000476966800025 ()
Funder
EU, European Research Council, 771777 FUN POLYSTORE
Available from: 2019-09-24 Created: 2019-09-24 Last updated: 2019-09-24Bibliographically approved
Qiu, Z., Shi, L., Wang, Z., Mindemark, J., Zhu, J.-F., Edström, K., . . . Yuan, S. (2019). Surface activated polyethylene separator promoting Li+ ion transport in gel polymer electrolytes and cycling stability of Li-metal anode. Chemical Engineering Journal, 368, 321-330
Open this publication in new window or tab >>Surface activated polyethylene separator promoting Li+ ion transport in gel polymer electrolytes and cycling stability of Li-metal anode
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2019 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 368, p. 321-330Article in journal (Refereed) Published
Abstract [en]

This paper proposes a strategy to fabricate surface activated polyethylene (PE)-supported gel polymer electrolyte (GPE) with high ion transport ability, excellent electrolyte retention and mechanical properties to stabilize lithium (Li)-metal anodes. The inert outer and inner pore surface activation of polyethylene is demonstrated by coating an ultrathin zirconium oxide nanocrystal (ZrO2)/polyhedral oligomeric silsesquioxane (POSS) composite layer through a simple layer by layer (LBL) assembly method prior to the in situ polymerization. It is found that the activation layer may improve the Li+ ion transference number and induce the formation of GPE with a gradient structure by the interaction with the initiator system, giving rise to higher ion transport ability of final GPE. On the other hand, the GPE using the activated PE separator as support improves the Li/electrolyte interfacial stability during storage and repeated lithium plating/stripping cycling. A stable voltage profile with cycling for more than 800 h in a Li/Li symmetric cell was obtained by using surface activated PE-supported GPE. When it is assembled into the cells with metallic lithium anodes and lithium cobalt oxide (LiCoO2) cathodes, the cells show excellent rate capability and cycling performance, as well as effective dendrite inhibition.

Keywords
Surface activation, Polyethylene support, Gel polymer electrolyte, Li-metal anode
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-382237 (URN)10.1016/j.cej.2019.02.107 (DOI)000462769600030 ()
Funder
Swedish Research Council
Available from: 2019-05-16 Created: 2019-05-16 Last updated: 2019-05-16Bibliographically approved
Sångeland, C., Younesi, R., Mindemark, J. & Brandell, D. (2019). Towards room temperature operation of all-solid-state Na-ion batteries through polyester-polycarbonate-based polymer electrolytes. ENERGY STORAGE MATERIALS, 19, 31-38
Open this publication in new window or tab >>Towards room temperature operation of all-solid-state Na-ion batteries through polyester-polycarbonate-based polymer electrolytes
2019 (English)In: ENERGY STORAGE MATERIALS, ISSN 2405-8297, Vol. 19, p. 31-38Article in journal (Refereed) Published
Abstract [en]

In an ambition to develop solid-state Na-ion batteries functional at ambient temperature, we here explore a novel electrolyte system. Polyester-polycarbonate (PCL-PTMC) copolymers were combined with sodium bis(fluorosulfonyl) imide salt (NaFSI) to form solid polymer electrolytes for Na-ion batteries. The PCL-PTMC:NaFSI system demonstrated glass transition temperatures ranging from -64 to -11 degrees C, increasing with increasing salt content from 0 to 35 wt%, and ionic conductivities ranging from 10(-8) to 10(-5) S cm(-1) at 25 degrees C. The optimal salt concentration was clearly dependent on the level of crystallinity, which was largely determined by the CL content. At 70 and 80 mol% CL, the PCL-PTMC:NaFSI system was fully amorphous and exhibited high conductivities at lower salt concentrations. When the CL content was increased to 100 mol%, high ionic conductivities were instead observed at high salt concentrations. A decent transference number of ca. 0.5 at 80 degrees C was obtained for a polymer film containing 20 mol% CL units and 25 wt% NaFSI. Finally, a HC vertical bar 80-20(25)vertical bar Na2-xFe(Fe(CN)(6)) all-solid-state polymer electrolyte full cell was assembled to demonstrate the practical application of the material and cycled for more than 120 cycles at similar to 22 degrees C.

Keywords
All-solid-state batteries, Solid polymer electrolyte, Room temperature cycling, Sodium-ion
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-387602 (URN)10.1016/j.ensm.2019.03.022 (DOI)000469207500004 ()
Funder
EU, European Research Council, 771777 FUN POLYSTORE
Available from: 2019-06-26 Created: 2019-06-26 Last updated: 2019-06-26Bibliographically approved
Xu, C., Hernández, G., Abbrent, S., Kober, L., Konefal, R., Brus, J., . . . Mindemark, J. (2019). Unraveling and Mitigating the Storage Instability of Fluoroethylene Carbonate-Containing LiPF6 Electrolytes To Stabilize Lithium Metal Anodes for High-Temperature Rechargeable Batteries. ACS APPLIED ENERGY MATERIALS, 2(7), 4925-4935
Open this publication in new window or tab >>Unraveling and Mitigating the Storage Instability of Fluoroethylene Carbonate-Containing LiPF6 Electrolytes To Stabilize Lithium Metal Anodes for High-Temperature Rechargeable Batteries
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2019 (English)In: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, no 7, p. 4925-4935Article in journal (Refereed) Published
Abstract [en]

Implementing Li metal anodes provides the potential of substantially boosting the energy density of current Li-ion battery technology. However, it suffers greatly from fast performance fading largely due to substantial volume change during cycling and the poor stability of the solid electrolyte interphase (SEI). Fluoroethylene carbonate (FEC) is widely acknowledged as an effective electrolyte additive for improving the cycling performance of batteries consisting of electrode materials that undergo large volume changes during cycling such as Li metal. In this study, we report that while FEC can form a robust SEI on the electrode, it also deteriorates the shelf life of electrolytes containing LiPF6. The degradation mechanism of LiPF6 in FEC solutions is unraveled by liquid-and solid-state NMR. Specifically, traces of water residues induce the hydrolysis of LiPF6, releasing HF and PF5 which further trigger ring-opening of FEC and its subsequent polymerization. These reactions are significantly accelerated at elevated temperatures leading to the formation of a three-dimensional fluorinated solid polymer network. Moisture scavenger additives, such as lithium 4,5-dicyano-2-(trifluoromethyl)imidazole (LiTDI), can delay the degradation reaction as well as improve the cycling stability of LiNi1/3Mn1/3Co1/3O2/Li metal batteries at 55 degrees C. This work highlights the poor shelf life of electrolytes containing FEC in combination with LiPF6 and thereby the great importance of developing proper storage methods as well as optimizing the content of FEC in practical cells.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
Keywords
lithium metal batteries, thermal instability, electrolyte storage instability, fluoroethylene carbonate, moisture scavenger, lithium 4, 5-dicyano-2-(trifluoromethyl)imidazole (LiTDI)
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-391950 (URN)10.1021/acsaem.9b00607 (DOI)000477074700040 ()
Funder
Swedish Energy Agency, 40466-1Swedish Energy Agency, 39043-1EU, Horizon 2020, 685716
Available from: 2019-08-29 Created: 2019-08-29 Last updated: 2019-08-29Bibliographically approved
Mindemark, J., Lacey, M. J., Bowden, T. & Brandell, D. (2018). Beyond PEO-Alternative host materials for Li+-conducting solid polymer electrolytes. Progress in polymer science, 81, 114-143
Open this publication in new window or tab >>Beyond PEO-Alternative host materials for Li+-conducting solid polymer electrolytes
2018 (English)In: Progress in polymer science, ISSN 0079-6700, E-ISSN 1873-1619, Vol. 81, p. 114-143Article, review/survey (Refereed) Published
Abstract [en]

The bulk of the scientific literature on Li-conducting solid (solvent-free) polymer electrolytes (SPEs) for applications such as Li-based batteries is focused on polyether-based materials, not least the archetypal poly(ethylene oxide) (PEO). A significant number of alternative polymer hosts have, however, been explored over the years, encompassing materials such as polycarbonates, polyesters, polynitriles, polyalcohols and polyamines. These display fundamentally different properties to those of polyethers, and might therefore be able to resolve the key issues restricting SPEs from realizing their full potential, for example in terms of ionic conductivity, chemical or electrochemical stability and temperature sensitivity. It is further interesting that many of these polymer materials complex Li-ions less strongly than PEO and facilitate ion transport through different mechanisms than polyethers, which is likely critical for true advancement in the area. In this review, >30 years of research on these 'alternative' Li-ion-conducting SPE host materials are summarized and discussed in the perspective of their potential application in electrochemical devices, with a clear focus on Li batteries. Key challenges and strategies forward and beyond the current PEO-based paradigm are highlighted.

Keywords
Polymer electrolyte, Solid electrolyte, Li battery, Ionic conductivity, Ion transport
National Category
Materials Chemistry Polymer Technologies
Identifiers
urn:nbn:se:uu:diva-365125 (URN)10.1016/j.progpolymsci.2017.12.004 (DOI)000433643500004 ()
Funder
Swedish Research Council, 2012-3837
Available from: 2018-11-12 Created: 2018-11-12 Last updated: 2018-11-12Bibliographically approved
Mindemark, J. (2018). Electrolytes for High-Performance Light-Emitting Electrochemical Cells: Going from Polyethers to Oligocarbonates. In: : . Paper presented at 16th International Symposium on Polymer Electrolytes, June 24 - 29, 2018 Yokohama Symposia, Yokohama, Japan.
Open this publication in new window or tab >>Electrolytes for High-Performance Light-Emitting Electrochemical Cells: Going from Polyethers to Oligocarbonates
2018 (English)Conference paper, Oral presentation with published abstract (Refereed)
National Category
Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:uu:diva-368335 (URN)
Conference
16th International Symposium on Polymer Electrolytes, June 24 - 29, 2018 Yokohama Symposia, Yokohama, Japan
Available from: 2018-12-04 Created: 2018-12-04 Last updated: 2019-03-07Bibliographically approved
Mindemark, J., Tang, S., Li, H. & Edman, L. (2018). Ion Transport beyond the Polyether Paradigm: Introducing Oligocarbonate Ion Transporters for Efficient Light-Emitting Electrochemical Cells. Advanced Functional Materials, 28(32), Article ID 1801295.
Open this publication in new window or tab >>Ion Transport beyond the Polyether Paradigm: Introducing Oligocarbonate Ion Transporters for Efficient Light-Emitting Electrochemical Cells
2018 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 28, no 32, article id 1801295Article in journal (Refereed) Published
Abstract [en]

The light-emitting electrochemical cell (LEC) is fundamentally dependent on mobile ions for its operation. In polymer LECs, the mobile ions are commonly provided by dissolving a salt in an ion transporter, with the latter almost invariably being an ether-based compound. Here, the synthesis, characterization, and application of a new class of carbonate-based ion transporters are reported. A polymer LEC, comprising a star-branched oligocarbonate endowed with aliphatic side groups as the ion transporter, features a current efficacy of 13.8 cd A(-1) at a luminance of 1060 cd m(-2), which is a record-high efficiency/luminance combination for a singlet-emitting LEC. It is further established that the design principles of a high-performance carbonate ion transporter constitute the selection of an oligomeric structure over a corresponding polymeric structure and the endowment of the oligomer with functional side chains to render it compatible with the polymeric emitter.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2018
Keywords
light emission, organic electronics, phase separation, polycarbonates, polymer electrolytes
National Category
Polymer Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-364983 (URN)10.1002/adfm.201801295 (DOI)000440810500004 ()
Funder
Swedish Foundation for Strategic Research Swedish Research CouncilSwedish Energy AgencyThe Kempe FoundationsKnut and Alice Wallenberg FoundationLars Hierta Memorial Foundation
Available from: 2018-11-07 Created: 2018-11-07 Last updated: 2018-11-16Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-9862-7375

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