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Reversibly compressible and freestanding monolithic carbon spherogels

2019, Salihovic, M., Zickler, G.A., Fritz-Popovski, G., Ulbricht, M., Paris, O., Hüsing, N., Presser, V., Elsaesser, M.S.

We present a versatile strategy to tailor the nanostructure of monolithic carbon aerogels. By use of an aqueous colloidal solution of polystyrene in the sol-gel processing of resorcinol-formaldehyde gels, we can prepare, after supercritical drying and successive carbonization, freestanding monolithic carbon aerogels, solely composed of interconnected and uniformly sized hollow spheres, which we name carbon spherogels. Each sphere is enclosed by a microporous carbon wall whose thickness can be adjusted by the polystyrene concentration, which affects the pore texture as well as the mechanical properties of the aerogel monolith. In this study, we used monodisperse polystyrene spheres of approximately 250 nm diameter, which result in an inner diameter of the final hollow carbon spheres of approximately 200 ± 5 nm due to shrinkage during the carbonization process. The excellent homogeneity of the samples, as well as uniform sphere geometries, are confirmed by small- and angle X-ray scattering. The presence of macropores between the hollow spheres creates a monolithic network with the benefit of being reversibly compressible up to 10% linear strain without destruction. Electrochemical tests demonstrate the applicability of ground and CO2 activated carbon spherogels as electrode materials. © 2019 The Authors

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High-performance ion removal via zinc–air desalination

2020, Srimuk, P., Wang, L., Budak, Ö., Presser, V.

Electrochemical processes enable a new generation of energy-efficient desalination technologies. While ion electrosorption via capacitive deionization is only suitable for brackish water with low molar strength, the use of Faradaic materials capable of reversible ion intercalation or conversion reactions allows energy-efficient removal of ions from seawater. However, the limited charge transfer/storage capacity of Faradaic materials indicates an upper limit for their desalination applications. Therefore, a new electrochemical concept must be explored to exceed the current state-of-the-art results and to push the desalination capacity beyond 100–200 mgNaCl/gelectrode. In this proof-of-concept work, we introduce the new concept of using metal–air battery technology for desalination. We do so by presenting performance data for zinc–air desalination (ZAD) in 600 mM NaCl. The ZAD cell provides a desalination capacity of 0.9–1.0 mgNaCl/cm2 (normalized to the membrane area; corresponding to 1300 mgNaCl/gZn) with a charge efficiency of 70% when charging/discharging the cell at 1 mA/cm2. The energy consumption of ZAD is 68–92 kJ/mol.

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Author Correction: Salt concentration and charging velocity determine ion charge storage mechanism in nanoporous supercapacitors

2019, Prehal, C., Koczwara, C., Amenitsch, H., Presser, V., Paris, O.

Correction to: Nature Communications; https://doi.org/10.1038/s41467-018-06612-4; published online 08 October 2018 The original version of this Article contained an error in the Acknowledgements, which was incorrectly omitted from the end of the following: ‘The research leading to these results has received funding from the European Community’s Horizon 2020 Framework Programme under grant agreement nº 730872.’ This has been corrected in both the PDF and HTML versions of the Article.

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Redox-electrolytes for non-flow electrochemical energy storage: A critical review and best practice

2019, Lee, J., Srimuk, P., Fleischmann, S., Su, X., Hatton, T.A., Presser, V.

Over recent decades, a new type of electric energy storage system has emerged with the principle that the electric charge can be stored not only at the interface between the electrode and the electrolyte but also in the bulk electrolyte by redox activities of the electrolyte itself. Those redox electrolytes are promising for non-flow hybrid energy storage systems, or redox electrolyte-aided hybrid energy storage (REHES) systems; particularly, when they are combined with highly porous carbon electrodes. In this review paper, critical design considerations for the REHES systems are discussed as well as the effective electrochemical characterization techniques. Appropriate evaluation of the electrochemical performance is discussed thoroughly, including advanced analytical techniques for the determination of the electrochemical stability of the redox electrolytes and self-discharge rate. Additionally, critical summary tables for the recent progress on REHES systems are provided. Furthermore, the unique synergistic combination of porous carbon materials and redox electrolytes is introduced in terms of the diffusion, adsorption, and electrochemical kinetics modulating energy storage in REHES systems. © 2018 The Author(s)

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Dual-Zinc Electrode Electrochemical Desalination

2020, Dai, J., Wang, J., Hou, X., Ru, Q., He, Q., Srimuk, P., Presser, V., Chen, F.

Continuous and low-energy desalination technologies are in high demand to enable sustainable water remediation. Our work introduces a continuous desalination process based on the redox reaction of a dual-zinc electrode. The system consists of two zinc foils as redox electrodes with flowing ZnCl2 electrolyte, concentrated and diluted salt streams with three anion- and cation-exchange membranes (AEM and CEM) separated configuration (AEM|CEM|AEM). If a constant current is applied, the negative zinc electrode is oxidized, and electrons are released to the external circuit, whereas the positive zinc electrode is reduced, causing salt removal in the dilution stream. The results showed that brackish water can be directly desalted to 380.6 ppm during a continuous batch-mode process. The energy consumption can be as low as 35.30 kJ mol−1 at a current density of 0.25 mA cm−2, which is comparable to reverse osmosis. In addition, the dual-zinc electrode electrochemical desalination demonstrates excellent rate performance, reversibility, and batch cyclability through electrode exchange regeneration. Our research provides a route for continuous low-energy desalination based on metal redox mediators.

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Low voltage operation of a silver/silver chloride battery with high desalination capacity in seawater

2019, Srimuk, P., Husmann, S., Presser, V.

Technologies for the effective and energy efficient removal of salt from saline media for advanced water remediation are in high demand. Capacitive deionization using carbon electrodes is limited to highly diluted salt water. Our work demonstrates the high desalination performance of the silver/silver chloride conversion reaction by a chloride ion rocking-chair desalination mechanism. Silver nanoparticles are used as positive electrodes while their chlorination into AgCl particles produces the negative electrode in such a combination that enables a very low cell voltage of only Δ200 mV. We used a chloride-ion desalination cell with two flow channels separated by a polymeric cation exchange membrane. The optimized electrode paring between Ag and AgCl achieves a low energy consumption of 2.5 kT per ion when performing treatment with highly saline feed (600 mM NaCl). The cell affords a stable desalination capacity of 115 mg g-1 at a charge efficiency of 98%. This performance aligns with a charge capacity of 110 mA h g-1. © The Royal Society of Chemistry.