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Chien, Y.-C., Pan, R., Lee, M.-T., Nyholm, L., Brandell, D. & Lacey, M. (2019). Cellulose Separators With Integrated Carbon Nanotube Interlayers for Lithium-Sulfur Batteries: An Investigation into the Complex Interplay between Cell Components. Journal of the Electrochemical Society, 166(14), A3235-A3241
Open this publication in new window or tab >>Cellulose Separators With Integrated Carbon Nanotube Interlayers for Lithium-Sulfur Batteries: An Investigation into the Complex Interplay between Cell Components
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2019 (English)In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 166, no 14, p. A3235-A3241Article in journal (Refereed) Published
Abstract [en]

This work aims to address two major roadblocks in the development of lithium-sulfur (Li-S) batteries: the inefficient deposition of Li on the metallic Li electrode and the parasitic "polysulfide redox shuttle". These roadblocks are here approached, respectively, by the combination of a cellulose separator with a cathode-facing conductive porous carbon interlayer, based on their previously reported individual benefits. Both approaches result in significant improvements in cycle life in test cells with positive electrodes with practically relevant specifications. Despite the substantially prolonged cycle life, the combination of the interlayer and cellulose separator generates an increase in polysulfide shuttle current, leading to greatly reduced Coulombic efficiency. Based on XPS analyses, the latter is ascribed to a change in the composition of the solid electrolyte interphase (SEI) on the Li electrode. At the same time, the rate of electrolyte decomposition is found to be lower in cells with cellulose-based separators, which corroborates the observation of longer cycle life. These seemingly contradictory and counterintuitive observations demonstrate the complicated interactions between the cell components in the Li-S system and how strategies aiming to mitigate one unwanted process may exacerbate another. This study demonstrates the value of a holistic approach to the development of Li-S chemistry.

National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-395795 (URN)10.1149/2.0301914jes (DOI)000487673900002 ()
Funder
Swedish Energy Agency, 42762-1Swedish Energy Agency, 42031-1
Available from: 2019-10-25 Created: 2019-10-25 Last updated: 2019-10-25Bibliographically approved
Zhou, S., Nyholm, L., Strømme, M. & Wang, Z. (2019). Cladophora Cellulose: Unique Biopolymer Nanofibrils for Emerging Energy, Environmental, and Life Science Applications. Accounts of Chemical Research, 52(8), 2232-2243
Open this publication in new window or tab >>Cladophora Cellulose: Unique Biopolymer Nanofibrils for Emerging Energy, Environmental, and Life Science Applications
2019 (English)In: Accounts of Chemical Research, ISSN 0001-4842, E-ISSN 1520-4898, Vol. 52, no 8, p. 2232-2243Article, review/survey (Refereed) Published
Abstract [en]

Conspectus

Because of its natural abundance, hierarchical fibrous structure, mechanical flexibility, potential for chemical modification, biocompatibility, renewability, and abundance, cellulose is one of the most promising green materials for a bio-based future and sustainable economy. Cellulose derived from wood or bacteria has dominated the industrial cellulose market and has been developed to produce a number of advanced materials for applications in energy storage, environmental, and biotechnology areas. However, Cladophora cellulose (CC) extracted from green algae has unprecedented advantages over those celluloses because of its high crystallinity (>95%), low moisture adsorption capacity, excellent solution processability, high porosity in the mesoporous range, and associated high specific surface area. The unique physical and chemical properties of CC can add new features to and enhance the performance of nanocellulose-based materials, and these attributes have attracted a great deal of research interest over the past decade.This Account summarizes our recent research on the preparation, characterization, functionalization, and versatile applications of CC. Our aim is to provide a comprehensive overview of the uniqueness of CC with respect to material structure, properties, and emerging applications. We discuss the potential of CC in energy storage, environmental science, and life science, with emphasis on applications in which its properties are superior to those of other nanocellulose forms. Specifically, we discuss the production of the first-ever paper battery based on CC. This battery has initiated a rising interest in the development of sustainable paper-based energy storage devices, where cellulose is used as a combined building block and binder for paper electrodes of various types in combination with carbon, conducting polymers, and other electroactive materials. High-active-mass and high-mass-loading paper electrodes can be made in which the CC acts as a high-surface-area and porous substrate while a thin layer of electroactive material is coated on individual nanofibrils. We have shown that CC membranes can be used directly as battery separators because of their low moisture content, high mesoporosity, high thermal stability, and good electrolyte wettability. The safety, stability, and capacity of lithium-ion batteries can be enhanced simply by using CC-based separators. Moreover, the high chemical modifiability and adjustable porosity of dried CC papers allow them to be used as advanced membranes for environmental science (water and air purification, pollutant adsorption) and life science (virus isolation, protein recovery, hemodialysis, DNA extraction, bioactive substrates). Finally, we outline some concluding perspectives on the challenges and future directions of CC research with the aim to open up yet unexplored fields of use for this interesting material.

National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-389512 (URN)10.1021/acs.accounts.9b00215 (DOI)000482534600019 ()31290643 (PubMedID)
Funder
Swedish Research CouncilSwedish Energy AgencyStiftelsen Olle Engkvist Byggmästare
Available from: 2019-07-16 Created: 2019-07-16 Last updated: 2019-10-04Bibliographically approved
Strömme, M., Mihranyan, A. & Nyholm, L. (2019). Composite materials including an intrinsically conducting polymer, and methods and devices. es ES08854650T.
Open this publication in new window or tab >>Composite materials including an intrinsically conducting polymer, and methods and devices
2019 (English)Patent (Other (popular science, discussion, etc.))
National Category
Nano Technology
Identifiers
urn:nbn:se:uu:diva-394123 (URN)
Patent
ES ES08854650T (2019-02-21)
Available from: 2019-10-03 Created: 2019-10-03 Last updated: 2019-10-03
Pan, R., Sun, R., Wang, Z., Lindh, J., Edström, K., Strömme, M. & Nyholm, L. (2019). Double-sided conductive separators for lithium-metal batteries. Energy Storage Materials, 21, 464-473
Open this publication in new window or tab >>Double-sided conductive separators for lithium-metal batteries
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2019 (English)In: Energy Storage Materials, ISSN 2405-8297, Vol. 21, p. 464-473Article in journal (Refereed) Published
Abstract [en]

A novel double-sided conductive (DSC) separator consisting of two 5 μm-thick carbon nanotube (CNT)/cellulose nanofiber (CNF) composite layers coated on each side of a 20 μm-thick glass-fiber (GF)/CNF composite membrane is described. In a lithium-metal battery (LMB), the DSC separator exhibits a high ionic conductivity (i.e. 1.7 mS cm−1 using an LP40 electrolyte) due to the high porosity (i.e. 66%) of the GF/CNF membrane. More stable Li anodes can also be realized by depositing Li within the porous electronically conducting CNT/CNF matrix at the DSC separator anode side due to the decreased current density. The CNT/CNF layer of the DSC separator facing the cathode, which is in direct electric contact with the current collector, decreases the overpotential for the cathode and consequently improves its capacity and rate performance significantly. A Li/Li cell containing a DSC separator showed an improved cycling stability compared to an analogous cell equipped with a commercial Celgard separator at current densities up to 5 mA cm−2 for Li deposition and stripping capacities up to 5 mAh cm−2. A proof-of-concept LMB containing a lithium iron phosphate (LFP) composite cathode and a DSC separator showed a significantly improved rate capability, yielding capacities of about 110 mAh g−1 at 5 C and 80 mAh g−1 at 10 C. The LMB cell containing a DSC separator also exhibited a capacity retention of 80% after 200 cycles at a rate of 6 C indicating that the two-sided conductive separator design has significant potential in facilitating the development of well-functioning LMBs.

Place, publisher, year, edition, pages
Elsevier, 2019
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-389860 (URN)10.1016/j.ensm.2019.06.025 (DOI)000484341600043 ()
Funder
Swedish Energy Agency
Available from: 2019-07-30 Created: 2019-07-30 Last updated: 2019-10-21Bibliographically approved
Xu, X., Makaraviciute, A., Abdurakhmanov, E., Werneling, F., Li, S., Danielson, U. H., . . . Zhang, Z. (2019). Estimating Detection Limits of Potentiometric DNA sensors Using Surface Plasmon Resonance Analyses.
Open this publication in new window or tab >>Estimating Detection Limits of Potentiometric DNA sensors Using Surface Plasmon Resonance Analyses
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2019 (English)In: Article in journal (Refereed) Submitted
National Category
Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:uu:diva-397806 (URN)
Funder
Swedish Foundation for Strategic Research , ICA 12-0047Swedish Foundation for Strategic Research , FFL15-0174Swedish Research Council, VR 2014-5588Wallenberg Foundations
Available from: 2019-11-25 Created: 2019-11-25 Last updated: 2019-11-26Bibliographically approved
Etman, A. S., Wang, Z., El Ghazaly, A., Sun, J., Nyholm, L. & Rosen, J. (2019). Flexible Freestanding MoO3-x-Carbon Nanotubes-Nanocellulose Paper Electrodes for Charge-Storage Applications. ChemSusChem
Open this publication in new window or tab >>Flexible Freestanding MoO3-x-Carbon Nanotubes-Nanocellulose Paper Electrodes for Charge-Storage Applications
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2019 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564XArticle in journal (Refereed) Epub ahead of print
Abstract [en]

Herein, a one-step synthesis protocol was developed for synthesizing freestanding/flexible paper electrodes composed of nanostructured molybdenum oxide (MoO3-x) embedded in a carbon nanotube (CNT) and Cladophora cellulose (CC) matrix. The preparation method involved sonication of the precursors, nanostructured MoO3-x, CNTs, and CC with weight ratios of 7:2:1, in a water/ethanol mixture, followed by vacuum filtration. The electrodes were straightforward to handle and possessed a thickness of approximately 12 mu m and a mass loading of MoO3-x-CNTs of approximately 0.9 mg cm(-2). The elemental mapping showed that the nanostructured MoO3-x was uniformly embedded inside the CNTs-CC matrix. The MoO3-x-CNTs-CC paper electrodes featured a capacity of 30 C g(-1), normalized to the mass of MoO3-x-CNTs, at a current density of 78 A g(-1) (corresponding to a rate of approximately 210 C based on the MoO3 content, assuming a theoretical capacity of 1339 C g(-1)), and exhibited a capacity retention of 91 % over 30 000 cycles. This study paves the way for the manufacturing of flexible/freestanding nanostructured MoO3-x-based electrodes for use in charge-storage devices at high charge/discharge rates.

Keywords
carbon nanotubes, charge storage applications, Cladophora cellulose, molybdenum oxide, paper electrodes
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-397673 (URN)10.1002/cssc.201902394 (DOI)000495103400001 ()31613052 (PubMedID)
Funder
Swedish Foundation for Strategic Research , EM16-0004Knut and Alice Wallenberg Foundation, KAW 2015.0043
Available from: 2019-11-28 Created: 2019-11-28 Last updated: 2019-11-28Bibliographically approved
Wang, Z., Tammela, P., Pan, R., Strömme, M. & Nyholm, L. (2019). Flexible Nanocellulose based Energy Storage Devices. In: MRS (Ed.), MRS Spring Meeting 2019: . Paper presented at MRS Spring Meeting 2019. Phoenix 22-26/4 2019. Phoenix, Article ID ES03.06.01ES03.06.01.
Open this publication in new window or tab >>Flexible Nanocellulose based Energy Storage Devices
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2019 (English)In: MRS Spring Meeting 2019 / [ed] MRS, Phoenix, 2019, article id ES03.06.01ES03.06.01Conference paper, Oral presentation with published abstract (Refereed)
Abstract [en]

The strong need for the development of inexpensive, flexible, light-weight and environmentally friendly energy storage devices has resulted in large interest in new cellulose-based electrode materials that can be used in batteries and supercapacitors [1-3]. In this presentation it will be shown that flexible nanocellulose and polypyrrole composites, manufactured by chemical polymerization of e.g. pyrrole on a nanocellulose substrate, can be used as electrodes in charge storage devices containing either water or organic solvent based electrolytes. The aqueous flexible paper-based devices exhibit high charge storage capacities (e.g. 9 Wh/kg) as well as excellent power capabilities (e.g. 3.5 kW/kg) due to the large surface area (up to 250 m2/g) of the nanocellulose and the thin (i.e. 50 nm) layer of polypyrrole present on the nanocellulose fibers. The straightforward (papermaking) composite synthesis approach and the electrochemical properties of the resulting composites will be discussed. It will also be shown that high active mass paper electrodes [4-8] with mass loadings of up to 20 mg/cm2 can be employed at high current densities without significant loss of electrochemical performance as a result of the advantageous structure of the electrodes. Devices with unprecedented areal and volumetric cell capacitances (e.g. 5.7 F/cm2 and 240 F/cm3) that can cycle for thousands of cycles in aqueous electrolytes can likewise be realized. As the cellulose composites also can be used in lithium-ion batteries [9,10], functional (e.g. redox-active) separators [11] for lithium based batteries and in the realization of all-cellulose energy storage devices [12], the present materials provide new exciting possibilities for the development of green and foldable devices for a range of new applications, many of which are incompatible with conventional batteries and supercapacitors.

Place, publisher, year, edition, pages
Phoenix: , 2019
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-389521 (URN)
Conference
MRS Spring Meeting 2019. Phoenix 22-26/4 2019
Available from: 2019-07-16 Created: 2019-07-16 Last updated: 2019-07-16
Zhao, J., Pan, R., Sun, R., Wen, C., Zhang, S.-L., Wu, B., . . . Zhang, Z.-B. (2019). High-Conductivity Reduced-Graphene-Oxide/Copper Aerogel for Energy Storage. Nano Energy, 60, 760-767
Open this publication in new window or tab >>High-Conductivity Reduced-Graphene-Oxide/Copper Aerogel for Energy Storage
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2019 (English)In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, Vol. 60, p. 760-767Article in journal (Refereed) Published
Abstract [en]

This work reports a room-temperature, solution-phase and one-pot method for macro-assembly of a three-dimensional (3D) reduced-graphene-oxide/copper hybrid hydrogel. The hydrogel is subsequently transformed into a highly conductive aerogel via freeze-drying. The aerogel, featuring reduced graphene oxide (rGO) networks decorated with Cu and CuxO nanoparticles (Cu/CuxO@rGO), exhibits a specific surface area of 48 m(2)/g and an apparent electrical conductivity of similar to 33 and similar to 430 S/m prior to and after mechanical compression, respectively. The compressed Cu/CuxO@rGO aerogel delivers a specific capacity of similar to 453 mAh g(-1) at a current density of 1 A/g and similar to 184 mAh g(-1) at 50 A/g in a 3 M KOH aqueous electrolyte evidenced by electrochemical measurements. Galvanostatic cycling tests at 5 A/g demonstrates that the Cu/CuxO@rGO aerogel retains 38% (similar to 129 mAh g(-1)) of the initial capacity (similar to 339 mAh g(-1)) after 500 cycles. The straightforward manufacturing process and the promising electrochemical performances make the Cu/CuxO@rGO aerogel an attractive electrode candidate in energy storage applications.

National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-381347 (URN)10.1016/j.nanoen.2019.04.023 (DOI)000467774100084 ()
Funder
Swedish Foundation for Strategic Research , Dnr SE13-0061Swedish Research Council, 621-2014-5596
Available from: 2019-04-08 Created: 2019-04-08 Last updated: 2019-06-11Bibliographically approved
Lindgren, F., Rehnlund, D., Pan, R., Pettersson, J., Younesi, R., Xu, C., . . . Nyholm, L. (2019). On the Capacity Losses Seen for Optimized Nano-Si Composite Electrodes in Li-Metal Half-Cells. Advanced Energy Materials, 9(33), Article ID 1901608.
Open this publication in new window or tab >>On the Capacity Losses Seen for Optimized Nano-Si Composite Electrodes in Li-Metal Half-Cells
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2019 (English)In: Advanced Energy Materials, ISSN 1614-6832, Vol. 9, no 33, article id 1901608Article in journal (Refereed) Published
Abstract [en]

While the use of silicon‐based electrodes can increase the capacity of Li‐ion batteries considerably, their application is associated with significant capacity losses. In this work, the influences of solid electrolyte interphase (SEI) formation, volume expansion, and lithium trapping are evaluated for two different electrochemical cycling schemes using lithium‐metal half‐cells containing silicon nanoparticle–based composite electrodes. Lithium trapping, caused by incomplete delithiation, is demonstrated to be the main reason for the capacity loss while SEI formation and dissolution affect the accumulated capacity loss due to a decreased coulombic efficiency. The capacity losses can be explained by the increasing lithium concentration in the electrode causing a decreasing lithiation potential and the lithiation cut‐off limit being reached faster. A lithium‐to‐silicon atomic ratio of 3.28 is found for a silicon electrode after 650 cycles using 1200 mAhg−1 capacity limited cycling. The results further show that the lithiation step is the capacity‐limiting step and that the capacity losses can be minimized by increasing the efficiency of the delithiation step via the inclusion of constant voltage delithiation steps. Lithium trapping due to incomplete delithiation consequently constitutes a very important capacity loss phenomenon for silicon composite electrodes.

Keywords
asymmetric cycling, hard X-ray photoelectron spectroscopy, lithium trapping, silicon, solid electrolyte interphase layer
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-398839 (URN)10.1002/aenm.201901608 (DOI)000477265600001 ()
Funder
Swedish Research Council, VR-2015-04421Swedish Research Council, VR-2017-06320StandUp
Note

De 2 första författarna delar förstaförfattarskapet.

Available from: 2019-12-11 Created: 2019-12-11 Last updated: 2019-12-11Bibliographically approved
Rehnlund, D., Ihrfors, C., Maibach, J. & Nyholm, L. (2019). Planar lithium: Electrochemical strategies circumventing dendritic lithium growth. Materials Today, 24, 119-120
Open this publication in new window or tab >>Planar lithium: Electrochemical strategies circumventing dendritic lithium growth
2019 (English)In: Materials Today, ISSN 1369-7021, E-ISSN 1873-4103, Vol. 24, p. 119-120Article in journal, Editorial material (Refereed) Published
Place, publisher, year, edition, pages
ELSEVIER SCI LTD, 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-382774 (URN)10.1016/j.mattod.2019.02.017 (DOI)000462777700025 ()
Funder
Swedish Research Council, VR. 2015-04421StandUp
Available from: 2019-05-02 Created: 2019-05-02 Last updated: 2019-05-02Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-9292-016X

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