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Rehnlund, D., Pettersson, J., Edström, K. & Nyholm, L. (2018). Lithium trapping in microbatteries based on lithium- and Cu2O-coated copper nanorods. ChemistrySelect, 3(8), 2311-2314
Open this publication in new window or tab >>Lithium trapping in microbatteries based on lithium- and Cu2O-coated copper nanorods
2018 (English)In: ChemistrySelect, E-ISSN 2365-6549, Vol. 3, no 8, p. 2311-2314Article in journal (Refereed) Published
Abstract [en]

Microbatteries based on three-dimensional (3D) electrodes composed of thin films of Li and Cu2O coated on Cu nanorod current collectors by electrodeposition and spontaneous oxidation, respectively, are described and characterised electrochemically. High-resolution scanning electron microscopy (HR-SEM) data indicate that the Li electrodeposition resulted in a homogenous coverage of the Cu nanorods and elemental analyses were also used to determine the amount of lithium in the Li-coated electrodes. The results show that 3D Cu2O/Cu electrodes can be cycled versus 3D Li/Cu electrodes but that the capacity decreased during the cycling due to Li trapping in the Cu current collector of the 3D Li/Cu electrode. These findings highlight the problem of using copper current collectors together with metallic lithium as the formation of a solid solution yields considerable losses of electroactive lithium and hence capacity.

Keywords
lithium trapping, microbatteries, nanorods, Cu2O, copper
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-343590 (URN)10.1002/slct.201800281 (DOI)000426495600015 ()
Funder
Swedish Research Council, 2012-4681, 2015-04421StandUpSwedish Energy Agency
Available from: 2018-02-28 Created: 2018-02-28 Last updated: 2018-05-31Bibliographically approved
Pan, R., Xu, X., Sun, R., Wang, Z., Lindh, J., Edström, K., . . . Nyholm, L. (2018). Nanocellulose Modified Polyethylene Separators for Lithium Metal Batteries. Small, 1-9, Article ID 1704371.
Open this publication in new window or tab >>Nanocellulose Modified Polyethylene Separators for Lithium Metal Batteries
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2018 (English)In: Small, p. 1-9, article id 1704371Article in journal (Refereed) Published
Abstract [en]

Abstract Poor cycling stability and safety concerns regarding lithium (Li) metal anodes are two major issues preventing the commercialization of high‐energy density Li metal‐based batteries. Herein, a novel tri‐layer separator design that significantly enhances the cycling stability and safety of Li metal‐based batteries is presented. A thin, thermally stable, flexible, and hydrophilic cellulose nanofiber layer, produced using a straightforward paper‐making process, is directly laminated on each side of a plasma‐treated polyethylene (PE) separator. The 2.5 µm thick, mesoporous (≈20 nm average pore size) cellulose nanofiber layer stabilizes the Li metal anodes by generating a uniform Li+ flux toward the electrode through its homogenous nanochannels, leading to improved cycling stability. As the tri‐layer separator maintains its dimensional stability even at 200 °C when the internal PE layer is melted and blocks the ion transport through the separator, the separator also provides an effective thermal shutdown function. The present nanocellulose‐based tri‐layer separator design thus significantly facilitates the realization of high‐energy density Li metal‐based batteries.

Keywords
cellulose, current distribution, lithium dendrites, lithium metal batteries, separators
National Category
Materials Chemistry Engineering and Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-349143 (URN)10.1002/smll.201704371 (DOI)
Available from: 2018-04-22 Created: 2018-04-22 Last updated: 2018-05-02Bibliographically approved
Wang, Z., Pan, R., Ruan, C., Edström, K., Strömme, M. & Nyholm, L. (2018). Redox-Active Separators for Lithium-Ion Batteries. ADVANCED SCIENCE, 5(3), Article ID 1700663.
Open this publication in new window or tab >>Redox-Active Separators for Lithium-Ion Batteries
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2018 (English)In: ADVANCED SCIENCE, ISSN 2198-3844, Vol. 5, no 3, article id 1700663Article in journal (Refereed) Published
Abstract [en]

A bilayered cellulose-based separator design is presented that can enhance the electrochemical performance of lithium-ion batteries (LIBs) via the inclusion of a porous redox-active layer. The proposed flexible redox-active separator consists of a mesoporous, insulating nanocellulose fiber layer that provides the necessary insulation between the electrodes and a porous, conductive, and redox-active polypyrrole-nanocellulose layer. The latter layer provides mechanical support to the nanocellulose layer and adds extra capacity to the LIBs. The redox-active separator is mechanically flexible, and no internal short circuits are observed during the operation of the LIBs, even when the redox-active layer is in direct contact with both electrodes in a symmetric lithium-lithium cell. By replacing a conventional polyethylene separator with a redox-active separator, the capacity of the proof-of-concept LIB battery containing a LiFePO4 cathode and a Li metal anode can be increased from 0.16 to 0.276 mA h due to the capacity contribution from the redox-active separator. As the presented redox-active separator concept can be used to increase the capacities of electrochemical energy storage systems, this approach may pave the way for new types of functional separators.

Place, publisher, year, edition, pages
WILEY, 2018
Keywords
capacity, cellulose, conducting polymers, lithium-ion batteries, redox-active separators
National Category
Materials Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-354519 (URN)10.1002/advs.201700663 (DOI)000428310500012 ()29593967 (PubMedID)
Funder
Swedish Foundation for Strategic Research , RMA-110012]Swedish Energy AgencyStandUpCarl Tryggers foundation
Available from: 2018-07-20 Created: 2018-07-20 Last updated: 2018-07-25Bibliographically approved
Wei, W., Valvo, M., Edström, K. & Nyholm, L. (2018). Size-dependent Electrochemical Performance of Monolithic Anatase TiO2 Nanotube Anodes for Sodium-ion Batteries. ChemElectroChem, 5(4), 674-684
Open this publication in new window or tab >>Size-dependent Electrochemical Performance of Monolithic Anatase TiO2 Nanotube Anodes for Sodium-ion Batteries
2018 (English)In: ChemElectroChem, Vol. 5, no 4, p. 674-684Article in journal (Refereed) Published
Abstract [en]

Well-defined, monolithic TiO2 nanotube thin films havebeen used as model anode electrodes to study Na-ion storage in anatase TiO2. It is shown that anatase TiO2 nanotubes with wall thicknesses up to 50 nm can be transformed into amorphous sodium titanate (e.g. Na0.2TiO2) nanotubes via an electrochemical activation process at about 0.2 V vs. Na+/Na. Due to the Na+ insertion and extraction reactions at about 0.55 and 0.75 V vs. Na+/Na, respectively, the activated TiO2 nanotubes exhibit reversible capacities of 170 mAh g-1. For the first time, it is shown that the nanotube length and wall thickness play critical roles in determining the electrochemical performances of this type of electrodes in Na-ion cells. An excellent rate performance, yielding capacities of about 33mAh g-1 at 20C and 161 mAh g-1 at C/5 rates, as well as a capacity retention of more than 97% after more than 350 cycles, could be achieved with nanotubes with a wall thickness of up to 20 nm. Thecycling rate for the nanotubes with a tube length of 4.5 μm should,however, be limited to 1C to guarantee a cycle life of about 200 cycles.

Keywords
TiO2, nanotubes, sodium, batteries, electrodes, free-standing, wall thickness, length
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-337289 (URN)10.1002/celc.201701267 (DOI)000425380200015 ()
Funder
Swedish Research Council Formas, 245- 2014-668StandUp
Available from: 2017-12-21 Created: 2017-12-21 Last updated: 2018-05-07Bibliographically approved
Malinovskis, P., Fritze, S., Riekehr, L., von Fieandt, L., Cedervall, J., Rehnlund, D., . . . Jansson, U. (2018). Synthesis and characterization of multicomponent (CrNbTaTiW)C films for increased hardness and corrosion resistance. Materials & design, 149, 51-62
Open this publication in new window or tab >>Synthesis and characterization of multicomponent (CrNbTaTiW)C films for increased hardness and corrosion resistance
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2018 (English)In: Materials & design, ISSN 0264-1275, E-ISSN 1873-4197, Vol. 149, p. 51-62Article in journal (Refereed) Published
Abstract [en]

Multicomponent carbide thin films of (CrNbTaTiW)C (30–40 at.% C) with different metal contents were depos-ited at different temperatures using non-reactive DC magnetron sputtering. The lattice distortion for the metallattice was estimated to vary from about 3 to 5%. Most films crystallized in the cubic B1 structure but Ta/W-rich films deposited at 600 °C exhibited a tetra gonal distortion. X-ray diffraction results sh ow that near-equimolar films exhibited a strong (111) texture. In contrast, Ta/W-rich films exhibited a shift from (111) to(100) texture at 450 °C. The in-plane relationship was determined to MC(111)[-12-1]//Al2O3(001)[110] with alattice mismatch of about 11% along the Al2O3[110] direction. A segregation of Cr to the grain boundaries was ob-served in all films. The microstructure was found to be the most important factor for high hardness. Less denseNb-rich and near-equimolar films deposited at low tem peratures exhib ited the low est hardnes s (12 GPa),while very dense Ta/W-rich high temperature films were found to be the hardest (36 GPa). No correlation wasfound between the lattice distortion and the hardness. Corrosion studies revealed that the multicomponentfilms exhibited excellent corrosion resistance, superior to that of a reference hyper-duplex stainless steel, in1.0 M HCl.

National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry; Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-335985 (URN)10.1016/j.matdes.2018.03.068 (DOI)000431007500006 ()
Funder
Swedish Research Council, 621-2012-4359Swedish Research Council, 622-2008-405Knut and Alice Wallenberg FoundationSwedish Foundation for Strategic Research , RMA11-0029
Available from: 2017-12-12 Created: 2017-12-12 Last updated: 2018-08-03Bibliographically approved
Oltean, G., Plylahan, N., Ihrfors, C., Wei, W., Chao, X., Edström, K., . . . Gustafsson, T. (2018). Towards Li-ion batteries operating at 80 °C: Ionic liquid versus conventional liquid electrolytes. Batteries, 4, 2-6, Article ID 10.3390/batteries4010002.
Open this publication in new window or tab >>Towards Li-ion batteries operating at 80 °C: Ionic liquid versus conventional liquid electrolytes
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2018 (English)In: Batteries, Vol. 4, p. 2-6, article id 10.3390/batteries4010002Article in journal (Refereed) Published
Abstract [en]

Li-ion battery (LIB) full cells comprised of TiO2-nanotube (TiO2-nt) and LiFePO4 (LFP)electrodes and either a conventional organic solvent based liquid electrolyte or an ionic liquid basedelectrolyte have been cycled at 80 °C. While the cell containing the ionic liquid based electrolyteexhibited good capacity retention and rate capability during 100 cycles, rapid capacity fading was found for the corresponding cell with the organic electrolyte. Results obtained for TiO2-nt and LFP half-cells indicate an oxidative degradation of the organic electrolyte at 80 °C. In all, ionic liquidbased electrolytes can be used to significantly improve the performance of LIBs operating at 80 °C.

Keywords
TiO2, ionic liquid, stability, elevated temperature, battery
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Materials Chemistry; Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-355542 (URN)10.3390/batteries4010002 (DOI)
Funder
Swedish Energy Agency, BatterifondenSwedish Foundation for Strategic Research , Road to Load
Available from: 2018-07-01 Created: 2018-07-01 Last updated: 2018-07-01
Sun, B., Asfaw, H. D., Rehnlund, D., Mindemark, J., Nyholm, L., Edström, K. & Brandell, D. (2018). Towards Solid-State 3D-Microbatteries using Functionalized Polycarbonate-based Polymer Electrolytes. ACS Applied Materials and Interfaces, 10(3), 2407-2413
Open this publication in new window or tab >>Towards Solid-State 3D-Microbatteries using Functionalized Polycarbonate-based Polymer Electrolytes
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2018 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 10, no 3, p. 2407-2413Article in journal (Refereed) Published
Abstract [en]

3D-microbatteries (3D-MBs) impose new demands for theselection, fabrication and compatibility of the different battery components, notleast the electrolytes. Herein, solid polymer electrolytes (SPEs) based on poly(trimethylene carbonate) (PTMC) have been implemented in 3D-MB systems. 3D electrodes of two different architectures, LiFePO4-coated carbon foams and Cu2O-coated Cu nanopillars, have been coated with SPEs and used in Li-cells. Functionalized PTMC with hydroxyl end groups was found to enable uniform and well-covering coatings on LiFePO4-coated carbon foams, although the cell cycling performance was limited by the large SPE resistance. By employing a SPE prepared from a copolymer of TMC and caprolactone (CL), with higher ionic conductivity, Li-cells composed of Cu2O-coated Cu nanopillars were constructed and tested both at room temperature and 60 °C. The footprint areal capacity of the cells was ca. 0.02 mAh cm-2 for an area gain factor (AF) of 2.5, and 0.2 mAh cm-2 for a relatively dense nanopillar-array (AF=25) at a current density of 0.008 mA cm-2at ambient temperature (22±1 °C). These results provide new routes towards the realization of all-solid-state 3D-MBs.

Keywords
Li-battery, 3D-microbattery, polymer electrolyte, nanopillars, carbon foam, Cu2O, Cu, nanorods
National Category
Inorganic Chemistry Materials Chemistry
Research subject
Chemistry with specialization in Organic Chemistry; Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-336964 (URN)10.1021/acsmi.7b13788 (DOI)000423496500027 ()29199816 (PubMedID)
Funder
StandUp
Available from: 2017-12-19 Created: 2017-12-19 Last updated: 2018-03-16Bibliographically approved
Lindgren, F., Rehnlund, D., Källquist, I., Nyholm, L., Edström, K., Hahlin, M. & Maibach, J. (2017). Breaking Down a Complex System: Interpreting PES Peak Positions for Cycled Li-ion Battery Electrodes. The Journal of Physical Chemistry C, 121, 27303-27312
Open this publication in new window or tab >>Breaking Down a Complex System: Interpreting PES Peak Positions for Cycled Li-ion Battery Electrodes
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2017 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, p. 27303-27312Article in journal (Refereed) Published
Abstract [en]

Photoelectron spectroscopy (PES) is an important technique for tracing and understanding the side reactions responsible for decreasing performance of Li-ion batteries. Interpretation of different spectral components is dependent on correct binding energy referencing and for battery electrodes this is highly complex. In this work, we investigate the effect on binding energy reference points in PES in correlation to solid electrolyte interphase (SEI) formation, changing electrode potentials and state of charge variations in Li-ion battery electrodes. The results show that components in the SEI have a significantly different binding energy reference point relative to the bulk electrode material (i.e. up to 2 eV). It is also shown that electrode components with electronically insulating/semi-conducting nature are shifted as a function of electrode potential relative to highly conducting materials. Further, spectral changes due to lithiation are highly depending on the nature of the active material and its lithiation mechanism. Finally, a strategy for planning and evaluating PES experiments on battery electrodes is proposed where some materials require careful choice of one or more internal reference points while others may be treated essentially without internal calibration.

National Category
Physical Sciences Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-336952 (URN)10.1021/acs.jpcc.7b08923 (DOI)000418393900008 ()
Funder
Swedish Energy Agency, 40495-1EU, FP7, Seventh Framework Programme, Eurolion & HiCSwedish Research Council, 2016-03545VINNOVA, High Voltage ValleyStandUp
Available from: 2017-12-19 Created: 2017-12-19 Last updated: 2018-02-16Bibliographically approved
Wang, Z., Tammela, P., Strömme, M. & Nyholm, L. (2017). Cellulose-based Supercapacitors: Material and Performance Considerations. Advanced Energy Materials, 7(18), Article ID 1700130.
Open this publication in new window or tab >>Cellulose-based Supercapacitors: Material and Performance Considerations
2017 (English)In: Advanced Energy Materials, ISSN 1614-6832, Vol. 7, no 18, article id 1700130Article in journal (Refereed) Published
Abstract [en]

One of the biggest challenges we will face over the next few decades is finding a way to power the future while maintaining strong socioeconomic growth and a clean environment. A transition from the use of fossil fuels to renewable energy sources is expected. Cellulose, the most abundant natural biopolymer on earth, is a unique, sustainable, functional material with exciting properties: it is low-cost and has hierarchical fibrous structures, a high surface area, thermal stability, hydrophilicity, biocompatibility, and mechanical flexibility, which makes it ideal for use in sustainable, flexible energy storage devices. This review focuses on energy storage applications involving different forms of cellulose (i.e., cellulose microfibers, nanocellulose fibers, and cellulose nanocrystals) in supercapacitors, with particular emphasis on new trends and performance considerations relevant to these fields. Recent advances and approaches to obtaining high capacity devices are evaluated and the limitations of cellulose-based systems are discussed. For the first time, a combination of device-specific factors such as electrode structures, mass loadings, areal capacities, and volumetric properties are taken into account, so as to evaluate and compare the energy storage performance and to better assess the merits of cellulose-based materials with respect to real applications.

Place, publisher, year, edition, pages
WILEY: Wiley-VCH Verlagsgesellschaft, 2017
Keywords
cellulose, supercapacitor
National Category
Materials Chemistry Polymer Chemistry Engineering and Technology
Research subject
Chemistry; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-333373 (URN)10.1002/aenm.201700130 (DOI)000411182500029 ()
Funder
Swedish Foundation for Strategic Research , RMA110012Stiftelsen Olle Engkvist ByggmästareSwedish Energy AgencyCarl Tryggers foundation
Available from: 2017-11-12 Created: 2017-11-12 Last updated: 2017-12-20Bibliographically approved
Böhme, S., Kerner, M., Scheers, J., Johansson, P., Edström, K. & Nyholm, L. (2017). Elevated Temperature Lithium-Ion Batteries Containing SnO2 Electrodes and LiTFSI-Pip14TFSI Ionic Liquid Electrolyte. Journal of the Electrochemical Society, 164(4), A701-A708
Open this publication in new window or tab >>Elevated Temperature Lithium-Ion Batteries Containing SnO2 Electrodes and LiTFSI-Pip14TFSI Ionic Liquid Electrolyte
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2017 (English)In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 164, no 4, p. A701-A708Article in journal (Refereed) Published
Abstract [en]

The performance of lithium-ion batteries (LIBs) comprising SnO2 electrodes and an ionic liquid (IL) based electrolyte, i.e., 0.5 MLiTFSI in Pip14TFSI, has been studied at room temperature (i.e., 22◦C) and 80◦C. While the high viscosity and low conductivity ofthe electrolyte resulted in high overpotentials and low capacities at room temperature, the SnO2 performance at 80◦C was found to beanalogous to that seen at room temperature using a standard LP40 electrolyte (i.e., 1MLiPF6 dissolved in 1:1 ethylene carbonate anddiethyl carbonate). Significant reduction of the IL was, however, found at 80◦C, which resulted in low coulombic efficiencies duringthe first 20 cycles, most likely due to a growing SEI layer and the formation of soluble IL reduction products. X-ray photoelectronspectroscopy studies of the cycled SnO2 electrodes indicated the presence of an at least 10 nm thick solid electrolyte interphase (SEI)layer composed of inorganic components such as lithium fluoride, sulfates, and nitrides as well as organic species containing C-H,C-F and C-N bonds.

National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-316877 (URN)10.1149/2.0861704jes (DOI)000400958600021 ()
Available from: 2017-03-07 Created: 2017-03-07 Last updated: 2017-06-14Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0001-9292-016X

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