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Schneider, S. F., Bauer, C., Novák, P. & Berg, E. (2019). A modeling framework to assess specific energy, costs and environmental impacts of Li-ion and Na-ion batteries. Sustainable Energy & Fuels
Open this publication in new window or tab >>A modeling framework to assess specific energy, costs and environmental impacts of Li-ion and Na-ion batteries
2019 (English)In: Sustainable Energy & FuelsArticle in journal (Refereed) Published
Abstract [en]

Li-ion batteries (LIBs) are among the most advanced technologies for energy storage. Due to the potential criticality of lithium raw materials, Na-ion batteries (NIBs) are frequently suggested as a low-cost, environmentally benign alternative to eventually complement or even replace LIBs. Herein, we present a holistic modeling framework to assess the potential of NIB cells from a performance, cost, and environmental impact perspective. To this end, we employ a physics-based battery cell model to project practical specific energies of LIB and NIB cells subjected to varying discharge rates. The derived performance metrics are subsequently used to parameterize a bottom-up battery cell cost model and to assess life cycle greenhouse gas (GHG) emission. Benchmarking model results obtained for NIBs (NaNi1/3Co1/3Mn1/3O2 vs. hard carbon) against state-of-the-art LIBs (LiNi1/3Co1/3Mn1/3O2 vs. graphite), we find that NIBs made from currently available active materials cannot compete with LIBs in terms of performance, costs, and environmental impact. Identifying battery performance as a key parameter driving manufacturing costs and GHG emissions, we argue that in order to make NIBs competitive to LIBs, one of the main priorities of NIB research should be the development of anode and cathode materials offering specific charges, voltages, and cycle life times comparable to or higher than for LIB active materials.

Place, publisher, year, edition, pages
The Royal Society of Chemistry, 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-392615 (URN)10.1039/C9SE00427K (DOI)
Available from: 2019-09-06 Created: 2019-09-06 Last updated: 2019-09-06
Kitz, P. G., Lacey, M., Novak, P. & Berg, E. (2019). Operando EQCM-D with Simultaneous in Situ EIS: New Insights into Interphase Formation in Li Ion Batteries. Analytical Chemistry, 91(3), 2296-2303
Open this publication in new window or tab >>Operando EQCM-D with Simultaneous in Situ EIS: New Insights into Interphase Formation in Li Ion Batteries
2019 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, no 3, p. 2296-2303Article in journal (Refereed) Published
Abstract [en]

An operando electrochemical quartz crystal microbalance with dissipation monitoring (EQCM-D) with simultaneous in situ electrochemical impedance spectroscopy (EIS) has been developed and applied to study the solid electrolyte interphase (SEI) formation on copper current collectors in Li-ion batteries. The findings are backed by EIS simulations and complementary analytical techniques, such as online electrochemical mass spectrometry (OEMS) and X-ray photoelectron spectroscopy (XPS). The evolution of mass and the mechanical properties of the SEI are directly correlated to the electrode impedance. Electrolyte reduction at the anode carbon active material initiates dissolution, diffusion, and deposition of reaction side products throughout the cell and increases electrolyte viscosity and the ohmic cell resistance as a result. On Cu the reduction of CuOx and HF occurs at >1.5 V and forms an initial LiF-rich interphase while electrolyte solvent reduction at <0.8 V vs Li+/Li adds a second, less rigid layer on top. Both the shear storage modulus and viscosity of the SEI generally increase upon cycling but-along with the SEI Li+ diffusion coefficient-also respond reversibly to electrode potential, likely as a result of Li+/EC interfacial concentration changes. Combined EIS-EQCM-D provides unique prospects for further studies of the highly dynamic structure-function relationships of electrode interphases in Li ion batteries.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
National Category
Physical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-378386 (URN)10.1021/acs.analchem.8b04924 (DOI)000458220300090 ()30569698 (PubMedID)
Available from: 2019-03-05 Created: 2019-03-05 Last updated: 2019-03-05Bibliographically approved
He, M., Fic, K., Frackowiak, E., Novak, P. & Jämstorp, E. (2019). Towards more Durable Electrochemical Capacitors by Elucidating the Ageing Mechanisms under Different Testing Procedures. CHEMELECTROCHEM, 6(2), 566-573
Open this publication in new window or tab >>Towards more Durable Electrochemical Capacitors by Elucidating the Ageing Mechanisms under Different Testing Procedures
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2019 (English)In: CHEMELECTROCHEM, ISSN 2196-0216, Vol. 6, no 2, p. 566-573Article in journal (Refereed) Published
Abstract [en]

Electrical double-layer capacitors (EDLCs) commonly denoted supercapacitors are rechargeable energy storage devices with excellent power and energy delivery metrics intermediate to conventional capacitors and batteries. High-voltage aqueous electrolyte based EDLCs are particularly attractive due to their high-power capability, facile production, and environmental advantages. EDLCs should last for thousands of cycles and evaluation of future cell chemistries require long-term and costly galvanostatic cycling. Voltage holding tests have been proposed to shorten evaluation time by accelerating cell degradation processes. Whether voltage holding can replace cycling completely remains undemonstrated. In this work, a systematic investigation of the influence of testing procedure on cell performance is presented. The state-of-the-art post-mortem and operando experimental techniques are implemented to elucidate ageing mechanisms and kinetics inside EDLC cells under different testing procedures. Carbon corrosion occurring on the positively polarized electrode leads to the lower active surface area and higher oxygen content. On the contrary, an increase of surface area and micropore volume are observed on the negatively polarized electrode. Repeated galvanostatic cycles at U<1.6 V appears to facilitate the depletion of oxygen species on the positively polarized electrode in comparison with voltage holding, which indicates a more complex degradation mechanism during cycling. Caution is advised when comparing results from different test procedures.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2019
Keywords
aqueous supercapacitors, cell ageing, cycling tests, high voltage, voltage holding
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-376830 (URN)10.1002/celc.201801146 (DOI)000456207200037 ()
Funder
EU, European Research Council, GA 759603
Available from: 2019-02-11 Created: 2019-02-11 Last updated: 2019-02-11Bibliographically approved
Flores, E., Vonrüti, N., Novák, P., Aschauer, U. & Berg, E. J. (2018). Elucidation of LixNi0.8Co0.15Al0.05O2 Redox Chemistry by Operando Raman Spectroscopy. Chemistry of Materials, 30(14), 4694-4703
Open this publication in new window or tab >>Elucidation of LixNi0.8Co0.15Al0.05O2 Redox Chemistry by Operando Raman Spectroscopy
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2018 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 30, no 14, p. 4694-4703Article in journal (Refereed) Published
Abstract [en]

The local structure evolution of LixNi0.8Co0.15Al0.05O2 (NCA) is linked to its electrochemical response during cycling (and overcharge) by operando Raman spectroscopy with findings supported by complementary techniques, such as online electrochemical mass spectrometry (OEMS) and density functional theory (DFT) phonon calculations. The vibrational motion of lattice oxygens is observed to be highly dependent on the local LixMO2 lattice environment, e.g. M—O bonding strength/length and state of lithiation x. All vibrational modes generally harden upon delithiation due to M—O bond character (ionic → covalent) evolution (disregarding an early bond softening due to Li+ vacancy formation) and evidence the important influence of the local structural lattice configuration on the electrochemical response of NCA. Although the intensities of all Raman active bands generally increase upon delithiation, a major inflection point at x = 0.2 marks the onset of a partly irreversible fundamental transition within NCA that is most likely related to electron removal from MO bonding states and partial oxidation of oxygen sublattice, which is also indicated by the observed concomitant O2 release from the particle surface. Operando Raman spectroscopy with higher time resolution provides unique possibilities for detailed studies of how chemical parameters (Li+ vacancy formation, transition metal cation concentration, and lattice doping, etc.) may govern the onset and nature of processes (such as bond character evolution and stability) that define the performance of the LixMO2 class of oxides. The further insights thus gained can be exploited to guide the development of next-generation layered cathodes for Li-ion batteries operating stably at higher voltages and capacities.

National Category
Condensed Matter Physics Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-364504 (URN)10.1021/acs.chemmater.8b01384 (DOI)000440105500026 ()
Available from: 2018-11-05 Created: 2018-11-05 Last updated: 2018-11-05Bibliographically approved
Flores, E., Novak, P. & Jämstorp, E. (2018). In situ and Operando Raman Spectroscopy of Layered Transition Metal Oxides for Li-ion Battery Cathodes. FRONTIERS IN ENERGY RESEARCH, 6, Article ID 82.
Open this publication in new window or tab >>In situ and Operando Raman Spectroscopy of Layered Transition Metal Oxides for Li-ion Battery Cathodes
2018 (English)In: FRONTIERS IN ENERGY RESEARCH, ISSN 2296-598X, Vol. 6, article id 82Article in journal (Refereed) Published
Abstract [en]

In situ and operando Raman spectroscopy is proposed to provide unique means for deeper fundamental understanding and further development of layered transition metal LiMO2 (M = Ni, Co, Mn) oxides suitable for Li-ion battery applications. We compare several spectro-electrochemical cell designs and suggest key experimental parameters for obtaining optimum electrochemical performance and spectral quality. Studies of the most practically relevant LiMO2 compositions are exemplified with particular focus on two experimental approaches: (1) lateral and axial Raman mapping of the electrode's (near-) surface to monitor inhomogeneous electrode reactions and (2) time-dependent single-particle spectra during cycling to analyze the LixMO2 lattice dynamics as a function of lithium content. Raman Spectroscopy is claimed to provide a unique real-time probe of the M-O bonds, which are at the heart of the electrochemistry of LiMO2 oxides and govern their stability. We highlight the need for further fundamental understanding of the relationships between the spectroscopic response and oxide lattice structure with particular emphasis on the development of a theoretical framework linking the position and intensity of the Raman bands to the local LixMO2 lattice con figuration. The use of complementary experimental techniques and model systems for validation also deserve further attention. Several novel LiMO2 compositions are currently being explored, especially containing dopings and coatings, and Raman spectroscopy could offer a highly dynamic and convenient tool to guide the formulation of high specific charge and long cycle life LiMO2 oxides for next-generation Li-ion battery cathodes.

Place, publisher, year, edition, pages
FRONTIERS MEDIA SA, 2018
Keywords
Raman spectroscopy, operando, in situ, LiMO2, Li-ion batteries, cathodes
National Category
Physical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-363936 (URN)10.3389/fenrg.2018.00082 (DOI)000442196200001 ()
Available from: 2018-10-24 Created: 2018-10-24 Last updated: 2018-11-05Bibliographically approved
Olsson, H., Berg, E. J., Strömme, M. & Sjödin, M. (2015). Self-discharge in positively charged polypyrrole-cellulose composite electrodes. Electrochemistry communications, 50, 43-46
Open this publication in new window or tab >>Self-discharge in positively charged polypyrrole-cellulose composite electrodes
2015 (English)In: Electrochemistry communications, ISSN 1388-2481, E-ISSN 1873-1902, Vol. 50, p. 43-46Article in journal (Refereed) Published
Abstract [en]

Self-discharge is one of the most critical issues to address to allow for industrialization of conducting polymer (CP) based electric energy storage devices. The present work investigates the underlying cause of self-discharge in positively charged polypyrrole (PPy), which is one of the most frequently studied CPs for such devices. The analyzed material is a composite of PPy and cellulose from Cladophora sp. algae forming a free standing paper-like material. From the time dependence of the potential decay as well as from independent spectroelectrochemical investigations the decay was attributed to a kinetically limiting Faradaic reaction, intrinsic to the polymer, forming a reactive intermediate that irreversibly reacts with its surroundings in a kinetically non-limiting following reaction. As such, nucleophilic addition of electrolyte nudeophiles is not found to be rate-determining. These results provide insight into the self-discharge phenomenon in p-doped CPs, and information regarding the potential range in which CPs can operate with insignificant self-discharge.

Keywords
Polypyrrole, Self-discharge, Activation-controlled Faradaic reaction, Stability, Maleimide, Degradation
National Category
Chemical Sciences Engineering and Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-245195 (URN)10.1016/j.elecom.2014.11.004 (DOI)000348260200011 ()
Available from: 2015-02-25 Created: 2015-02-25 Last updated: 2018-11-05Bibliographically approved
Olsson, H., Sjödin, M., Jämstorp Berg, E., Strømme, M. & Nyholm, L. (2014). Self-discharge Reactions in Energy Storage Devices Based on Polypyrrole-cellulose Composite Electrodes. Green, 4(1-6), 27-39
Open this publication in new window or tab >>Self-discharge Reactions in Energy Storage Devices Based on Polypyrrole-cellulose Composite Electrodes
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2014 (English)In: Green, ISSN 1869-8778, Vol. 4, no 1-6, p. 27-39Article in journal (Refereed) Published
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-238205 (URN)10.1515/green-2014-0003 (DOI)1869-8778 1869-876X (ISBN)
Available from: 2014-12-10 Created: 2014-12-10 Last updated: 2018-11-05
Karlsson, C., Jämstorp, E., Strømme, M. & Sjödin, M. (2012). Computational Electrochemistry Study of 16 Isoindole-4,7-diones as Candidates for Organic Cathode Materials. The Journal of Physical Chemistry C, 116(5), 3793-3801
Open this publication in new window or tab >>Computational Electrochemistry Study of 16 Isoindole-4,7-diones as Candidates for Organic Cathode Materials
2012 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 116, no 5, p. 3793-3801Article in journal (Refereed) Published
Abstract [en]

Prediction of the redox behavior of electroactive molecules enables screening of a variety of compounds and can serve as a guideline in the search for organic molecules for use as cathode materials in, for example, Li ion batteries. In this study, we present a computational strategy, based on density functional theory, to calculate redox potentials and acid dissociation constants for a series of 16 isoindole-4,7-dione (IID) derivatives. The calculations take all possible electron and proton transfers into account, and the results were found to correlate very well with electrochemical and spectroscopic measurements. The possibility of polymerizing the IID derivatives was also assessed computationally, as polymerization serves as a straightforward route to immobilize the active material. Three of the considered IIDs (5,6-dicyano-2-methyl-isoindole-4,7-dione, 5,6-dihydroxy-2-methyl-isoindole-4,7-dione, and 2-methyl-5-(trifluoromethyl)-isoindole-4,7-dione) are predicted to be particularly interesting for making polymers for organic cathodes because these are calculated to have high redox potentials and high specific capacities and to be readily polymerizable. The presented strategy is general and can be applied in the prediction of the electrochemical behavior of quinones as well as other systems involving proton and electron transfers.

Place, publisher, year, edition, pages
American Chemical Society, 2012
National Category
Other Chemistry Topics Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-168889 (URN)10.1021/jp211851f (DOI)000299985300073 ()
Available from: 2012-02-17 Created: 2012-02-17 Last updated: 2018-11-05Bibliographically approved
Jämstorp Berg, E. (2012). Diffusion Controlled Drug Release from Slurry Formed, Porous, Organic and Clay-derived Pellets. (Doctoral dissertation). Uppsala: Acta Universitatis Upsaliensis
Open this publication in new window or tab >>Diffusion Controlled Drug Release from Slurry Formed, Porous, Organic and Clay-derived Pellets
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Coronary artery disease and chronic pain are serious health issues that cause severe discomfort and suffering in society today. Antithrombotic agents and highly potent analgesics play a critical role in improving the recovery process for patients being treated for these diseases. This thesis focuses on the design and study of pellet-based drug dosage forms which allow diffusion-controlled delivery of drugs with the aim of achieving optimal therapeutic outcomes.

A wet slurry process was used to mix the drug and the polymer and/or clay precursor excipients into a paste. The pellets were then shaped via ionotropic gelation (alginate hydrogel beads/pellets), extrusion/spheronization (halloysite clay pellets) or geopolymerization.

The decrease in the drug diffusion rate in the alginate beads was affected by the drug's molecular size and charge and the characteristics (such as concentration and chemical structure) of the surrounding alginate gel.

The halloysite clay pellets provided sustained release of the highly potent drug fentanyl at both gastric pH 1 and intestinal pH 6.8. As expected, crushing the pellets reduced the diffusion barrier, resulting in more rapid release (dose dumping).

The use of mechanically strong geopolymer gels was investigated as a potential means of preventing dose dumping as a result of crushing of the dosage form. Variations in the synthesis composition resulted in drastic changes in the microstructure morphology, the porosity, the mechanical stability and the drug release rate. Pore network modeling and finite element simulations were employed to theoretically evaluate the effects of porosity and drug solubility in the geopolymer structure on the drug release process. Fitting the model parameters to experimental data showed that increased average pore connectivity, a greater pore size distribution, and increased drug solubility in the pellet resulted in an increased drug release rate. Furthermore, incorporation of pH-sensitive organic polymers in the geopolymer structure reduced the high drug release rate from the pellets at gastric pH. These results indicate that geopolymers have potential for use in pellet form; both the release rate of the drug and the mechanical stability of the pellets can be optimized to prevent dose dumping.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2012. p. 80
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 884
Keywords
Diffusion, Drug delivery, Antithrombotic drugs, Highly potent opioids, Modeling, Clays, Polymers, Pellets, Beads
National Category
Pharmaceutical Sciences
Research subject
Materials Science
Identifiers
urn:nbn:se:uu:diva-161812 (URN)978-91-554-8229-9 (ISBN)
Public defence
2012-01-20, Häggsalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:00 (English)
Opponent
Supervisors
Available from: 2011-12-21 Created: 2011-11-17 Last updated: 2018-11-05
Jämstorp, E., Strømme, M. & Bredenberg, S. (2012). Influence of drug distribution and solubility on release from geopolymer pellets: A finite element method study. Journal of Pharmaceutical Sciences, 101(5), 1803-1810
Open this publication in new window or tab >>Influence of drug distribution and solubility on release from geopolymer pellets: A finite element method study
2012 (English)In: Journal of Pharmaceutical Sciences, ISSN 0022-3549, E-ISSN 1520-6017, Vol. 101, no 5, p. 1803-1810Article in journal (Refereed) Published
Abstract [en]

This study investigates the influence of drug solubility and distribution on its release from inert geopolymer pellets of three different sizes (1.5 × 1.5, 3 × 6, and 6 × 6 mm), having the same geopolymer composition and containing highly potent opioid fentanyl, sumatriptan, theophylline, or saccharin. Scanning electron microscopy, nitrogen sorption, drug solubility, permeation, and release experiments were performed, and estimates of the drug diffusion coefficients and solubilities in the geopolymer matrix were derived with the aid of finite element method (FEM). FEM was further employed to investigate the effect of a nonuniform drug distribution on the drug release profile. When inspecting the release profiles for each drug, it was observed that their solubilities in the geopolymer matrix imposed a much greater influence on the drug release rate than their diffusion coefficients. Concentrating the initial drug load in FEM into nonuniformly distributed drug regions inside the matrix created drug release profiles that more closely resembled experimental data than an FEM-simulated uniform drug distribution did. The presented FEM simulations and visualization of drug release from geopolymers under varying initial and dynamic conditions should open up for more systematic studies of additional factors that influence the drug release profile from porous delivery vehicles.

Keywords
controlled release, solubility, diffusion, dissolution, materials science, oral drug delivery
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Engineering Science with specialization in Materials Science
Identifiers
urn:nbn:se:uu:diva-161810 (URN)10.1002/jps.23071 (DOI)000302800100016 ()
Available from: 2011-11-17 Created: 2011-11-17 Last updated: 2018-11-05Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-5653-0383

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