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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
Rehnlund, D., Ihrfors, C., Maibach, J. & Nyholm, L. (2018). Dendrite-free lithium electrode cycling via controlled nucleation in low LiPF6 concentration electrolytes. Materials Today, 21(10), 1010-1018
Open this publication in new window or tab >>Dendrite-free lithium electrode cycling via controlled nucleation in low LiPF6 concentration electrolytes
2018 (English)In: Materials Today, ISSN 1369-7021, E-ISSN 1873-4103, Vol. 21, no 10, p. 1010-1018Article in journal (Refereed) Published
Abstract [en]

Lithium metal electrodes are not widely used in rechargeable batteries as dendritic lithium growth and electrolyte reactions raise serious stability and safety concerns. In this study, we show that reproducible two-dimensional lithium deposition can be realized using a lithium salt concentration of 0.020 M, an added supporting salt, and a short lithium nucleation pulse. This approach, which is common in electrodeposition of metals, increases the lithium nuclei density on the electrode surface and decreases the extent of Li+ migration favoring dendritic lithium growth. Contrary to common belief, ascribing the dendrite problem to heterogeneous lithium nucleation due to an unstable solid electrolyte interphase layer, we show that the main lithium deposition problem stems from the difficulty to obtain two-dimensional deposition at the low lithium deposition overpotentials encountered in conventional high-lithium concentration electrolytes. The present results hence clearly demonstrate that two-dimensional lithium deposition can be realized in lithium-metal-based batteries.

Keywords
Two-dimensional, Metallic nanocrystals, Renewable energy, Electrocatalysis
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-372816 (URN)10.1016/j.mattod.2018.08.003 (DOI)000452551100017 ()
Funder
Swedish Research Council, VR. 2015-04421StandUp
Available from: 2019-01-09 Created: 2019-01-09 Last updated: 2019-01-14Bibliographically approved
Rehnlund, D., Ihrfors, C. & Nyholm, L. (2018). Electrochemical Manufacturing and Characterisation of Nanostructured Electrodes for Lithium based Batteries. In: : . Paper presented at The 233rd ECS Meeting, May 13-17 2018, Seattle, USA.
Open this publication in new window or tab >>Electrochemical Manufacturing and Characterisation of Nanostructured Electrodes for Lithium based Batteries
2018 (English)Conference paper, Oral presentation with published abstract (Other academic)
Abstract [en]

Due to their high energy and power densities, lithium-ion batteries are the primary choice for application in consumer electronics. Although new electrode materials for Li-ion batteries are developed continuously, relatively little attention has so far been paid to the use of electrochemical methods in the manufacturing of battery materials. In the field of microbatteries, electrodeposition has, nevertheless, become an important technique for the manufacturing of current collectors, electrode materials and electrolytes [1]. During the last few years it has also been shown that electrochemically nanostructured electrodes lacking binders and other additives can facilitate the attainment of an improved understanding of the electrochemical reactions taking place in lithium based batteries.  

This presentation will focus on the development of electrochemical approaches for the manufacturing and study of nanostructured electrode materials for lithium based batteries. It will be shown that electrodeposition can be used for the manufacturing of 3-D copper and aluminium [1] current collectors as well as the coating of these with thin layers of anode or cathode materials. Electrochemical manufacturing and characterisation of materials such as multilayered Cu/Cu2O nanorods [2], Sn/SnO2 particles [3] and TiO2 nanotubes (see Figure 1) will be discussed, as well as a new approach for the manufacturing of TiO2 nanotube size gradient based electrodes [4]. Some fundamental issues regarding the electrochemical processes in the electrochemically manufactured materials, including the formation of “cathodic passive layers” and “trapping of lithium” in current collectors and alloy forming electrode materials [5] and the electrodeposition of homogeneous lithium films on lithium electrodes (see Figure 1) will likewise be discussed.

 

 

References

 

[1]   K. Edström, D. Brandell, T. Gustafsson, L. Nyholm, Electrodeposition as a tool for 3D Microbattery Fabrication, Electrochem. Soc. Interface, 20 (2011) 41.

[2]   D. Rehnlund, M. Valvo, C. –W. Tai, J. Ångström, M. Sahlberg, K. Edström, L. Nyholm, Electrochemical fabrication and characterization of Cu/Cu2O multi-layered micro and nanorods in Li-ion batteries, Nanoscale, 7 (2015) 13591.

[3]   S. Böhme, K. Edström, L. Nyholm, Overlapping and Rate Controlling Electrochemical Reactions for Tin(IV) Oxide Electrodes in Lithium-Ion Batteries, J. Electroanal. Chem., 797 (2017) 47.

[4]   W. Wei, F. Björefors, L. Nyholm, Hybrid energy storage devices based on monolithic electrodes containing well-defined TiO2 nanotube size gradients, Electrochim. Acta, 176 (2015) 1393.

Keywords
electrodeposition, nanostructured electrodes, diffusion, trapping, alloy formation, conversion reactions, intercalation, TiO2, silicon, tin, lithium deposition
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry; Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-355547 (URN)
Conference
The 233rd ECS Meeting, May 13-17 2018, Seattle, USA
Funder
Swedish Research Council, 2015-04421
Available from: 2018-07-01 Created: 2018-07-01 Last updated: 2018-10-31Bibliographically approved
Rehnlund, D., Lindgren, F., Pettersson, J., Edström, K. & Nyholm, L. (2018). Lithium Trapping in Alloy forming Electrodes and Current Collectors for Lithium based Batteries. In: : . Paper presented at The 233rd ECS Meeting, Seattle, USA, May 13-17 2018.
Open this publication in new window or tab >>Lithium Trapping in Alloy forming Electrodes and Current Collectors for Lithium based Batteries
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2018 (English)Conference paper, Oral presentation with published abstract (Other academic)
Abstract [en]

The next generation of lithium based batteries can be expected to be based on lithium alloy forming anode materials which can store up to ten times more charge than the currently used graphite anodes. This increase in the charge storage capability has motivated significant research towards the commercialization of anode materials such as Si, Sn and Al. These alloy forming anode materials are, however, known to exhibit significant capacity losses during cycling. This is typically ascribed to the volume expansion associated with the formation of the lithium alloys (the volume expansion is e.g. about 280 % for Li3.75Si) resulting in electrode pulverization as well as continuous solid electrolyte interphase (SEI) layer formation [1-3]. While significant progress has been made to decrease the volume expansion problems by the use of e.g. nanoparticles, nanorods and thin films, and/or capacity limitations [1-3], capacity losses are still generally seen [4,5]. This and previously published data suggest that the phenomenon may be due to another effect and that this in fact could stem from lithium trapping in the electrodes [6-8].

In the present work it is demonstrated (based on e.g. elemental analyses of cycled Sn, Al and Si electrodes) that lithium trapping can account for the capacity losses seen when alloy forming anode materials are cycled versus lithium electrodes, see Figure 1. It is shown that small amounts of elemental lithium are trapped within the electrode material during the cycling as a result of a two-way diffusion process [8] causing the lithium to move into the bulk material even during the delithiation step. This phenomenon, which can be explained by the lithium concentration profiles in the electrodes, makes a complete delithiation process very time consuming. As a result of the lithium trapping effect, the lithium concentration in the electrode increases continuously during the cycling. The experimental results also show that a similar effect can be seen also for commonly used current collector metals such as Cu, Ni and Ti. The latter means that these metals are unsuitable as current collector materials for lithium alloy forming materials in the absence of a thin layer of boron doped diamond serving as a lithium diffusion barrier layer [8].

References

1    M. N. Obrovac and V. L. Chevrier, Chem. Rev., 2014, 114, 11444.

2    X. Su, Q. Wu, J. Li, X. Xiao, A. Lott, W. Lu, B. W. Sheldon and J. Wu, Adv. Energy Mater., 2014, 4, 1300882.

3    J. R. Szczech and S. Jin, Energy Environ. Sci., 2011, 4, 56.

4    G. Zheng, S. W. Lee, Z. Liang, H-W. Lee, K. Yan, H. Yao, H. Wang, W. Li, S. Chu and Y. Cui, Nat. Nanotechnol., 2014, 9, 618.

5    K. Yan, H-W. Lee, T. Gao, G. Zheng, H. Yao, H. Wang, Z. Lu, Y. Zhou, Z. Liang, Z. Liu, S. Chu and Y. Cui, Nano Letters, 2014, 14, 6016.

6    G. Oltean, C-W. Tai, K. Edström and L. Nyholm, J. Power Sources, 2014, 269, 266.

7    A. L. Michan, G. Divitini, A. J. Pell, M. Leskes, C. Ducati and C. P. Grey, J. Am. Chem. Soc., 2016, 138, 7918.

8    D. Rehnlund, F. Lindgren, S. Böhme, T. Nordh, Y. Zou, J. Pettersson, U. Bexell, M. Boman, K. Edström and L. Nyholm, Energy Environ. Sci., 10 (2017) 1350.

 

Keywords
Lithium, trapping, diffusion, alloy formation, silicon, tin, aluminium
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry; Chemistry with specialization in Materials Chemistry; Chemistry with specialization in Organic Chemistry; Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-355546 (URN)
Conference
The 233rd ECS Meeting, Seattle, USA, May 13-17 2018
Funder
Swedish Research Council, 2015-04421
Available from: 2018-07-01 Created: 2018-07-01 Last updated: 2018-10-31Bibliographically approved
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
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
Pan, R., Xu, X., Sun, R., Wang, Z., Lindh, J., Edström, K., . . . Nyholm, L. (2018). Nanocellulose Modified Polyethylene Separators for Lithium Metal Batteries. Small, 14(21), 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, ISSN 1613-6810, E-ISSN 1613-6829, Vol. 14, no 21, 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.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2018
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)000434173300006 ()29675952 (PubMedID)
Funder
Swedish Foundation for Strategic Research , RMA-110012Swedish Energy AgencyStandUp
Available from: 2018-04-22 Created: 2018-04-22 Last updated: 2018-12-10Bibliographically approved
Wang, Z., Pan, R., Sun, R., Edström, K., Strömme, M. & Nyholm, L. (2018). Nanocellulose Structured Paper-Based Lithium Metal Batteries. ACS Applied Energy Materials, 1(8), 4341-4350
Open this publication in new window or tab >>Nanocellulose Structured Paper-Based Lithium Metal Batteries
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2018 (English)In: ACS Applied Energy Materials, Vol. 1, no 8, p. 4341-4350Article in journal (Refereed) Published
Abstract [en]

We report for the first time, a lithium metal battery (LMB) design based on low-cost, renewable, and mechanically flexible nanocellulose fibers (NCFs) as the separator as well as substrate materials for both the positive and negative electrodes. Combined with carbon nanofibers, the NCFs yield 3D porous conducting cellulose paper (CCP) current collectors with large surface areas, enabling a low effective current density. The porous structure yields a dendrite-free deposition of lithium (Li), faciliates the mass transport within the electrodes, and also compensates for the volume changes during the cycling. Stable Li electrodes are obtained by electrodepositing Li on CCP substrates while positive electrodes are realized by embedding LiFePO4 (LFP) particles within the flexible CCP matrix. The mesoporous NCF separator features a homogeneous pore distribution which provides uniform current distributions at the electrodes. This effect, which yields a more homogeneous Li deposition on the negative electrode as well as improves the safety, lifespan, and sustainability of the LMB. As a result, the present all-nanocellulose-based LMB demonstrates excellent cycling stability for a Li metal battery obtained to date, with 91% capacity retention after 800 cycles and 85% capacity retention after 1000 cycles at a rate of 2 C (i.e., 1.27 mA cm–2).

Place, publisher, year, edition, pages
American Chemical Society, 2018
National Category
Inorganic Chemistry Materials Chemistry Engineering and Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-358031 (URN)10.1021/acsaem.8b00961 (DOI)
Available from: 2018-08-23 Created: 2018-08-23 Last updated: 2018-12-10Bibliographically approved
Etman, A., Wang, L., Nyholm, L., Edström, K. & Sun, J. (2018). One-pot Synthesis of MoO3-x Nanosheets for Supercapacitor Applications. In: : . Paper presented at The E-MRS 2018 Spring Meeting, June 18 to 22, Strasbourg, France.
Open this publication in new window or tab >>One-pot Synthesis of MoO3-x Nanosheets for Supercapacitor Applications
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2018 (English)Conference paper, Oral presentation with published abstract (Other academic)
Abstract [en]

Molybdenum oxide nanosheets are interesting materials for energy storage, catalysis, and gas sensor applications.1 However, they are traditionally prepared via a variety of approaches which require the use of high temperature or organic solvents.2,3 Herein, we report the synthesis of MoO3-x nanosheets (where x denotes oxygen vacancy) via a one-step water based exfoliation strategy using bulk molybdenum oxides precursors.4 Scanning and transmission electron microscopy show that the MoO3-x has a typical nanosheet morphology with a few nanometer thickness. The MoO3-x nanosheets display localized surface plasmon resonance (LSPR), which can be enhanced by modifying the morphology and the amount of oxygen vacancies (x) using chemical and/or photochemical treatments.

The aqueous suspension of the MoO3-x nanosheets was drop-cast onto carbon paper and this material was then used as binder free electrodes for supercapacitor applications. The electrodes showed promising performance regarding capacitance and rate capability in acidified sodium sulphate solutions. The facile green synthesis of MoO3-x nanosheets coupled with their significant photochemical and electrochemical properties pave the way for the use of the nanosheets in a variety of applications.

References:

(1)        de Castro, I. A.; Datta, R. S.; Ou, J. Z.; Castellanos-Gomez, A.; Sriram, S.; Daeneke, T.; Kalantar-zadeh, K. Molybdenum Oxides - From Fundamentals to Functionality. Adv. Mater. 2017, 29 (40), 1701619.

(2)        Xiao, X.; Song, H.; Lin, S.; Zhou, Y.; Zhan, X.; Hu, Z.; Zhang, Q.; Sun, J.; Yang, B.; Li, T.; Jiao, L.; Zhou, J.; Tang, J.; Gogotsi, Y. Scalable Salt-Templated Synthesis of Two-Dimensional Transition Metal Oxides. Nat. Commun. 2016, 7, 11296.

(3)        Alsaif, M. M. Y. A.; Field, M. R.; Daeneke, T.; Chrimes, A. F.; Zhang, W.; Carey, B. J.; Berean, K. J.; Walia, S.; van Embden, J.; Zhang, B.; Latham, K.; Kalantar-zadeh, K.; Ou, J. Z. Exfoliation Solvent Dependent Plasmon Resonances in Two-Dimensional Sub-Stoichiometric Molybdenum Oxide Nanoflakes. ACS Appl. Mater. Interfaces 2016, 8 (5), 3482–3493.

(4)      Etman A. S.; Abdelhamid H. N.; Yuan Y.; Wang L.; Zou X.; Sun J. Facile Water Based Strategy for Synthesizing MoO3-x Nanosheets: Efficient Visible Light Photocatalyst for Dye Degradation. ACS Omega. in Press.

Keywords
synthesis, MoO3-x, nanosheets, supercapacitor
National Category
Inorganic Chemistry
Research subject
Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-355552 (URN)
Conference
The E-MRS 2018 Spring Meeting, June 18 to 22, Strasbourg, France
Available from: 2018-07-01 Created: 2018-07-01 Last updated: 2018-11-01Bibliographically approved
Tammela, P., Yamada, S., Wang, Z., Strømme, M. & Nyholm, L. (2018). Paper based electrodes suitable for disposable packaging. In: Intelligent and Connected Packaging Solutions: . Paper presented at Smart Packaging, Hamburg, 9-10 October, 2018.
Open this publication in new window or tab >>Paper based electrodes suitable for disposable packaging
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2018 (English)In: Intelligent and Connected Packaging Solutions, 2018Conference paper, Oral presentation only (Refereed)
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-366096 (URN)
Conference
Smart Packaging, Hamburg, 9-10 October, 2018
Available from: 2018-11-16 Created: 2018-11-16 Last updated: 2018-11-26
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-9292-016X

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