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- Schäfer, David, et al.
(author)
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Multiscale Investigation of Sodium-Ion Battery Anodes: Analytical Techniques and Applications
- 2024
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In: Advanced Energy Materials. - 1614-6840 .- 1614-6832. ; 14:15
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Journal article (peer-reviewed)abstract
- The anode/electrolyte interface behavior, and by extension, the overall cell performance of sodium-ion batteries is determined by a complex interaction of processes that occur at all components of the electrochemical cell across a wide range of size- and timescales. Single-scale studies may provide incomplete insights, as they cannot capture the full picture of this complex and intertwined behavior. Broad, multiscale studies are essential to elucidate these processes. Within this perspectives article, several analytical and theoretical techniques are introduced, and described how they can be combined to provide a more complete and comprehensive understanding of sodium-ion battery (SIB) performance throughout its lifetime, with a special focus on the interfaces of hard carbon anodes. These methods target various length- and time scales, ranging from micro to nano, from cell level to atomistic structures, and account for a broad spectrum of physical and (electro)chemical characteristics. Specifically, how mass spectrometric, microscopic, spectroscopic, electrochemical, thermodynamic, and physical methods can be employed to obtain the various types of information required to understand battery behavior will be explored. Ways are then discussed how these methods can be coupled together in order to elucidate the multiscale phenomena at the anode interface and develop a holistic understanding of their relationship to overall sodium-ion battery function.
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- Seidel, Y.E., et al.
(author)
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Mesoscopic mass transport effects in electrocatalytic processes
- 2008
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In: Faraday Discussions. - : Royal Society of Chemistry (RSC). - 1359-6640 .- 1364-5498. ; 140, s. 167-184
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Journal article (peer-reviewed)abstract
- The role of mesoscopic mass transport and re-adsorption effects in electrocatalytic reactions was investigated using the oxygen reduction reaction (ORR) as an example. The electrochemical measurements were performed on structurally well-defined nanostructured model electrodes under controlled transport conditions in a thin-layer flow cell. The electrodes consist of arrays of Pt ultra-microelectrodes (nanodisks) of defined size (diameter similar to 100 nm) separated on a planar glassy carbon (GC) substrate, which were fabricated employing hole-mask colloidal lithography (HCL). The measurements reveal a distinct variation in the ORR selectivity with Pt nanodisk density and with increasing electrolyte flow, showing a pronounced increase of the H2O2 yield, by up to 65%, when increasing the flow rate from 1 to 30 mu L s(-1). These results are compared with previous findings and discussed in terms of a reaction model proposed recently (A. Schneider et al., Phys. Chem. Chem. Phys., 2008, 10, 1931), which includes (i) direct reduction to H2O on the Pt surface and (ii) additional H2O2 formation and desorption on both Pt and carbon surfaces and subsequent partial re-adsorption and further reduction of the H2O2 molecules on the Pt surface. The potential of model studies on structurally defined catalyst surfaces and under well-defined mass transport conditions in combination with simulations for the description of electrocatalytic reactions is discussed.
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- Seidel, Y.E., et al.
(author)
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Mesoscopic transport effects in electrocatalytic reactions
- 2009
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In: ECS Transactions. - : The Electrochemical Society. - 1938-5862 .- 1938-6737. - 9781566777902 ; 25:23, s. 91-102
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Conference paper (peer-reviewed)abstract
- Transport effects may not only influence the rate of electrocatalytic reactions, but also the product distribution. The underlying effects were studied under well-defined reaction and transport conditions, using nanostructured Pt/glassy carbon electrodes, which consist of ordered arrays of electrocatalytically active Pt nanostructures on a planar glassy carbon substrate. The effect of varying the density of the Pt nanostructures or the electrolyte flow rate on the reaction characteristics and product distribution was investigated for apparently simple electrocatalytic reactions such as CO oxidation, methanol oxidation and oxygen reduction. It is shown that reducing the Pt coverage leads to an increase of the relative amount of the reaction intermediates. Similar effects are obtained for increasing the electrolyte flow rate. The results are discussed on a molecular scale in terms of the 'desorption - re-adsorption - reaction' model which we had introduced recently.
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- Seidel, Y. E., et al.
(author)
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Nanostructured Pt/GC model electrodes prepared by the deposition of metal-salt-loaded micelles
- 2007
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In: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 23:10, s. 5795-5801
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Journal article (peer-reviewed)abstract
- Novel, nanostructured, carbon-supported Pt model electrodes with homogeneously distributed Pt nanoparticles of uniform size were fabricated and analyzed with respect to their electrochemical properties. For this purpose, Pt-salt-loaded micelles were deposited on a glassy carbon substrate and subsequently exposed to an oxygen plasma and a H-2 atmosphere for removal of the polymer carriers and reduction of the Pt salt. The morphology of the resulting nanoparticles and their electrochemical/electrocatalytic properties were characterized by high-resolution scanning electron microscopy, X-ray photoelectron spectroscopy, cyclic voltammetry, and differential electrochemical mass spectrometry for CO electrooxidation. The data demonstrate that this method is generally suited to the production of nanostructured model electrodes with well-defined and independently adjustable particle size and interparticle distance distributions, which are specifically suited for quantitative studies of transport processes in electrocatalytic reactions.
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- Seidel, Y. E., et al.
(author)
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Stability of nanostructured Pt/glassy carbon electrodes prepared by colloidal lithography
- 2008
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In: Journal of the Electrochemical Society. - : The Electrochemical Society. - 0013-4651 .- 1945-7111. ; 155:3, s. K50-K58
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Journal article (peer-reviewed)abstract
- The stability of nanostructured Pt/glassy carbon (GC) model electrodes upon exposure to a realistic electrochemical/electrocatalytic reaction environment (continuous reaction, continuous electrolyte flow) was studied by microscopic techniques, X-ray photoelectron spectroscopy, and electrochemical measurements. The model electrodes consist of Pt nanostructures with well-defined sizes and regular spacing on planar GC substrates, and were fabricated using colloidal lithography techniques. Additional plasma treatments of the GC substrates prior to Pt deposition were tested to improve the stability of the resulting Pt/GC model electrodes. Both evaporation and sputter deposition were used for Pt-film fabrication. The model catalysts prepared by Pt evaporation were found to be rather unstable. The stability was significantly improved for sputter-deposited Pt films, and Pt sputter deposition on a GC substrate, pretreated first in oxygen plasma and then in Ar plasma, resulted in stable model electrodes with a fully intact layer of Pt nanostructures after the electrocatalytic experiments.
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