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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
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
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
Pan, R., Wang, Z., Sun, R., Lindh, J., Edström, K., Strömme, M. & Nyholm, L. (2019). Polydopamine-based redox-active separators for lithium-ion batteries. Journal of Materiomics, 204-213
Open this publication in new window or tab >>Polydopamine-based redox-active separators for lithium-ion batteries
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2019 (English)In: Journal of Materiomics, ISSN 2352-8478, p. 204-213Article in journal (Refereed) Published
Abstract [en]

The performance of lithium-ion batteries (LIBs) can be effectively increased with functionalized separators. Herein, it is demonstrated that polydopamine-based redox-active (PRA) separators can provide additional capacity to that of typical anode materials, increase the volumetric capacity of the cell, as well as, decrease the cell resistance to yield an improved performance at higher cycling rates. The PRA separators, which are composed of a 2 μm thick electrically insulating nanocellulose fiber (NCF) layer and an 18 μm thick polydopamine (PDA) and carbon nanotube (CNT) containing redox-active layer, are readily produced using a facile paper-making process. The PRA separators are also easily wettable by commonly employed electrolytes (e.g. LP40) and exhibit a high dimensional stability. In addition, the pore structure endows the PRA separator with a high ionic conductivity (i.e. 1.06 mS cm−1) that increases the rate performance of the cells. Due to the presence of the redox-active layer, Li4Ti5O12 (LTO) half-cells containing PRA separator were found to exhibit significantly higher capacities than the corresponding cells containing commercial separators. These results clearly show that the implementation of this type of redox-active separators constitutes a straightforward and effective way to increase the energy and power densities of LIBs.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Lithium-ion battery, Separator, Cellulose, Polydopamine, Redox-active
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-370069 (URN)10.1016/j.jmat.2018.12.007 (DOI)000470660000008 ()
Funder
Swedish Energy Agency, 2017-013543
Available from: 2018-12-18 Created: 2018-12-18 Last updated: 2019-06-26Bibliographically approved
Pan, R., Sun, R., Wang, Z., Lindh, J., Edström, K., Strömme, M. & Nyholm, L. (2019). Sandwich-structured nano/micro fiber-based separators for lithium metal batteries. Nano Energy, 55, 316-326
Open this publication in new window or tab >>Sandwich-structured nano/micro fiber-based separators for lithium metal batteries
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2019 (English)In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, Vol. 55, p. 316-326Article in journal (Refereed) Published
Abstract [en]

Although the increased need for high-energy/power-density energy storage systems has revived the research on lithium metal batteries (LMBs), the influence of the separator on the performance of LMBs is still generally neglected. In the present study, a sandwich-structured separator (referred to as the CGC separator below) composed of two 2.5µm thick cellulose nanofiber (CNF) surface layers and an intermediate 15µm thick glass microfiber (GMF) and CNF composite layer is described. While the CNF surface layers of the CGC separator feature a homogeneous distribution of nano-sized pores favoring the attainment of a homogeneous current distribution at both electrodes, the intermediate GMF/CNF layer contains macropores facilitating the ionic transport through the separator. The CGC separator exhibited a much better electrolyte wettability and thermal stability compared to a Celgard separator, due to the use of the hydrophilic and thermally stable CNFs and GMFs. It is also shown that the combination of nano-sized and micro-sized fibers used in the CGC separator yields a higher ionic conductivity than that for the commercial separator (1.14 vs. 0.49 mS cm−1). Moreover, the influence of the separator pore structure (e.g. the porosity and pore distribution) on the performance of LMBs is studied for both Li anodes and LiFePO4 composite cathodes. The results demonstrate that the use of separators with high porosities and homogeneous surface pore distributions can improve the performances (e.g. capacities and stabilities) of LMBs considerably, and also highlights the importance of proper separator/electrode interactions. The present approach constitutes a practical engineering strategy for the production of separators with nano/micro fibers and a promising route for the development of LMBs with improved safety and enhanced electrochemical performances.

Keywords
Cellulose, separator, sandwich structure, lithium metal battery, current distribution, three-electrode
National Category
Nano Technology Materials Chemistry
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-364826 (URN)10.1016/j.nanoen.2018.11.005 (DOI)000454636200029 ()
Funder
StandUpSwedish Energy Agency
Available from: 2018-11-04 Created: 2018-11-04 Last updated: 2019-06-12Bibliographically approved
Ruan, C., Wang, Z., Lindh, J. & Strömme, M. (2018). Carbonized cellulose beads for efficient capacitive energy storage. Cellulose (London), 25(6), 3545-3556
Open this publication in new window or tab >>Carbonized cellulose beads for efficient capacitive energy storage
2018 (English)In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 25, no 6, p. 3545-3556Article in journal (Refereed) Published
Abstract [en]

Natural biomaterials, including polysaccharides and amino acids, provide a sustainable source of functional carbon materials for electric energy storage applications. We present a one-pot reductive amination process to functionalize 2,3-dialdehyde cellulose (DAC) beads with chitosan and l-cysteine to provide single (N)- and dual (N/S)-doped materials. The functionalization enables the physicochemical properties of the materials to be tailored and can provide carbon precursors with heteroatom doping suitable for energy storage applications. Scanning electron microscopy, Fourier transform infrared spectroscopy and thermogravimetric analysis were used to characterize the changes to the beads after functionalization and carbonization. The results of X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy verified that the doping was effective, while the nitrogen sorption isotherms and pore-size distributions of the carbonized beads showed the effects of doping with different hierarchical porosities. In the electrochemical experiments, three kinds of carbon beads [pyrolyzed from DAC, chitosan-crosslinked DAC (CS-DAC) and l-cysteine-functionalized DAC] were used as electrode materials. Electrodes of carbonized CS-DAC beads had a specific capacitance of up to 242 F g(-1) at a current density of 1 A g(-1). These electrodes maintained a capacitance retention of 91.5% after 1000 charge/discharge cycles, suggesting excellent cycling stability. The results indicate that reductive amination of DAC is an effective route for heteroatom doping of carbon materials to be used as electrode active materials for energy storage.

Keywords
2, 3-Dialdehyde cellulose (DAC) beads, Nitrogen doping, Nitrogen/sulfur doping, Supercapacitor
National Category
Materials Chemistry Physical Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-357553 (URN)10.1007/s10570-018-1811-6 (DOI)000432990300030 ()
Funder
Swedish Foundation for Strategic Research Stiftelsen Olle Engkvist Byggmästare
Available from: 2018-08-17 Created: 2018-08-17 Last updated: 2018-08-17Bibliographically approved
Wang, Z., Li, M., Ruan, C., Liu, C., Zhang, C., Xu, C., . . . Nyholm, L. (2018). Conducting Polymer Paper-Derived Mesoporous 3D N-doped Carbon Current Collectors for Na and Li Metal Anodes: A Combined Experimental and Theoretical Study. The Journal of Physical Chemistry C, 122(41), 23352-23363
Open this publication in new window or tab >>Conducting Polymer Paper-Derived Mesoporous 3D N-doped Carbon Current Collectors for Na and Li Metal Anodes: A Combined Experimental and Theoretical Study
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2018 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, no 41, p. 23352-23363Article in journal (Refereed) Published
Abstract [en]

Herein, the manufacturing of a free-standing N-doped mesoporous carbon (CPPY) paper by straightforward carbonization of polypyrrole-coated nanocellulose paper is described. The deposition of Na and Li on these CPPY electrodes, which also serve as current collectors, is studied using a combination of experiments and theoretical calculations. The porous CPPY electrodes gave rise to decreased current densities, which helped to prolong the life-time of the Na electrodes. While the density functional theory calculations suggest that both Na and Li should be deposited uniformly on the CPPY electrodes, the experimental results clearly show that the sodium deposition was more well-defined on the surface of the CPPY electrodes. In contrast to Li, dendrite-free Na depositions could be carried out using deposition capacities up to 12 mAh cm(-2 )and a stable Na electrode cycling performance was found during 1000 h at 1 mA cm(-2). The results suggest that it was difficult to predict the Na or Li deposition behavior merely based on calculations of the metal adsorption energies, as kinetic effects should also be taken into account. Nevertheless, the experimental results clearly show that the use of the present type of porous electrodes provides new possibilities for the development of durable Na electrodes for high-performance sodium metal batteries.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2018
National Category
Materials Chemistry Physical Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-369911 (URN)10.1021/acs.jpcc.8b07481 (DOI)000448087900013 ()
Funder
Swedish Energy AgencyeSSENCE - An eScience Collaboration
Available from: 2018-12-17 Created: 2018-12-17 Last updated: 2019-01-02Bibliographically approved
Wang, Z., Pan, R., Xu, C., Ruan, C., Edström, K., Strømme, M. & Nyholm, L. (2018). Conducting polymer paper-derived separators for lithium metal batteries. Energy Storage Materials, 13, 283-292
Open this publication in new window or tab >>Conducting polymer paper-derived separators for lithium metal batteries
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2018 (English)In: Energy Storage Materials, ISSN 2405-8297, Vol. 13, p. 283-292Article in journal (Refereed) Published
Abstract [en]

Overoxidised polypyrrole (PPy) paper has been employed as a mesoporous separator for lithium metal batteries (LMBs) based on its narrow pore size distribution, good thermal stability, high ionic conductivity (1.1 mS cm−1 with a LP40 electrolyte) and high electrolyte wettability. The overoxidised PPy paper was produced from a PPy/cellulose composite using a combined base and heat-treatment process, yielding a highly interrupted pyrrole molecular structure including N-containing polar groups maintaining the readily adaptable mesoporous structure of the pristine PPy paper. This well-defined pore structure gave rise to a homogeneous current distribution which significantly increased the performance of a LiFePO4|Li cell. With the overoxidised PPy separator, a symmetric Li|Li cell could be cycled reversibly for more than 600 h without any short-circuits in a LP40 electrolyte. This approach facilitates the manufacturing of well-defined separators for fundamental investigations of the influence of the separator structure on the performance of LMBs.

Keywords
Conducting polymers, nanocellulose, separator, porosity, lithium metal, batteries
National Category
Inorganic Chemistry Engineering and Technology
Research subject
Chemistry with specialization in Inorganic Chemistry; Chemistry with specialization in Materials Chemistry; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-355543 (URN)10.1016/j.ensm.2018.02.006 (DOI)000436924800033 ()
Funder
Swedish Energy Agency, TriLiSwedish Foundation for Strategic Research , RMA-110012Carl Tryggers foundation StandUp
Available from: 2018-07-01 Created: 2018-07-01 Last updated: 2018-09-13Bibliographically approved
Wang, Z., Zhang, X., Zhou, S., Edström, K., Strömme, M. & Nyholm, L. (2018). Lightweight, Thin, and Flexible Silver Nanopaper Electrodes for High-Capacity Dendrite-Free Sodium Metal Anodes. Advanced Functional Materials, 28(48), Article ID 1804038.
Open this publication in new window or tab >>Lightweight, Thin, and Flexible Silver Nanopaper Electrodes for High-Capacity Dendrite-Free Sodium Metal Anodes
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2018 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 28, no 48, article id 1804038Article in journal (Refereed) Published
Abstract [en]

Owing to its resource-abundant and favorable theoretical capacity, sodium metal is regarded as a promising anode material for sodium metal batteries. However, uncontrolled Na plating/stripping, including Na dendrite growth during cycling, has hindered its practical application. Herein, a sodiophilic, thin, and flexible silver nanopaper (AgNP) is designed based on interpenetrated nanocellulose and silver nanowires and is used as a dendrite-free Na metal electrode. Due to a network of highly conducting silver nanowire (0.6 Ω sq?1, 8200 S cm?1), the sodiophilic nature of silver, and the reduced internal strain within the flexible AgNP, a compact Na metal layer can be uniformly deposited on and reversibly stripped from the AgNP electrode without any observations of Na dendrites during cycling at 1 mA cm?2 for 800 h. As the AgNP electrode is only 2 µm thick, with a low mass loading of 0.88 mg cm?2, the AgNP?Na anode deposited with a Na deposition charge of 6 mAh cm?2 exhibits a capacity of 995 mAh g?1AgNP?Na, approaching that of a Na metal anode (1166 mAh g?1Na). The present approach provides new possibilities for the development of lightweight and stable metal batteries.

Place, publisher, year, edition, pages
Wiley-Blackwell, 2018
Keywords
dendrite-free electrodes, flexible electrodes, silver nanowires, sodiophilc, sodium metal anodes
National Category
Nano Technology Materials Chemistry
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-364853 (URN)10.1002/adfm.201804038 (DOI)000451118800003 ()
Funder
Swedish Energy AgencyStandUp
Available from: 2018-11-05 Created: 2018-11-05 Last updated: 2019-01-25Bibliographically approved
Wang, Z., Tammela, P., Strömme, M. & Nyholm, L. (2018). Nanocellulose based energy storage devices. Paper presented at 255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water, March 18-22 2018, New Orleans, USA. Abstract of Papers of the American Chemical Society, 255
Open this publication in new window or tab >>Nanocellulose based energy storage devices
2018 (English)In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 255Article in journal, Meeting abstract (Other academic) Published
Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
National Category
Other Materials Engineering Medical Materials
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-349147 (URN)000435537702530 ()
Conference
255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water, March 18-22 2018, New Orleans, USA
Available from: 2018-04-22 Created: 2018-04-22 Last updated: 2018-12-12Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-6118-0226

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