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  • Dimitrakopoulos, Georgios  (3)
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  • 1
    Online Resource
    Online Resource
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-02, No. 40 ( 2020-11-23), p. 2574-2574
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-02, No. 40 ( 2020-11-23), p. 2574-2574
    Abstract: Increasing the performance of Solid Oxide Electrolysis Cells (SOECs) for the production of hydrogen (H 2 ) from water (H 2 O) splitting requires the use of cathodes with low polarization resistance. In-situ growth of metal catalysts from perovskite oxides (termed catalyst exsolution) has been proposed as a means to decorate the porous electrode with highly dispersed, nanometer-sized catalytic particles [1-3]. These particles are highly active towards reactions of interest and show increased resistance to agglomeration due to their socketed nature [4] . In this work, we investigate the in-situ , on demand exsolution of catalysts by using fuel and electrochemistry as a means to decrease the temperature and duration required to grow catalytic particles on the surface of electrodes. We study the performance, stability, particle morphology and distribution as a function of electrochemical polarization applied at the electrode. Substantial improvement of reaction kinetics is found, consistent with previous reports [5]. In addition, we probe the effect of electrochemical and temperature conditions on the particle size, shape and distribution. In addition, we propose tuning the reducibility of parent oxides to be a good strategy in controlling the size and dispersion of the exsolved particles, and demonstrate this approach on epitaxial perovskite thin films. Moreover, our observations suggest oxygen vacancies to be the potential nucleation sites of the exsolved particles. The present study provides a new direction towards the generation of nanoparticle-size catalysts on the surface of perovskite oxides given the increasing demand for active and durable catalysts in the field of solid oxide cells and in other energy and fuels conversion processes. References: [1] G. Tsekouras et. al. Energy Environ. Sci., 2013, 6, 256–266 [2] Y. Sun et. al. J. Mater. Chem. A, 2015, 3, 11048–11056 [3] G. Dimitrakopoulos et. al. Sustainable Energy & Fuels 2019, 3, 2347-2355 [4] D. Neagu et. al. Nature Communications 8:1855 (2017) [5] J. Myung et. al. Nature 537 (2016) 528-531
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2020
    detail.hit.zdb_id: 2438749-6
    Location Call Number Limitation Availability
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  • 2
    Online Resource
    Online Resource
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-01, No. 36 ( 2020-05-01), p. 1473-1473
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-01, No. 36 ( 2020-05-01), p. 1473-1473
    Abstract: Increasing the performance of Solid Oxide Electrolysis Cells (SOECs) for the production of hydrogen (H 2 ) from water (H 2 O) splitting requires the use of cathodes with low polarization resistance. In-situ growth of metal catalysts from perovskite oxides (termed catalyst exsolution) has been proposed as a means to decorate the porous electrode with highly dispersed, nanometer-sized catalytic particles [1-3]. These particles are highly active towards reactions of interest and show increased resistance to agglomeration due to their socketed nature [4] . In this work, we investigate the in-situ , on demand exsolution of catalysts by using fuel and electrochemistry as a means to decrease the temperature and duration required to grow catalytic particles on the surface of electrodes. We study the performance, stability, particle morphology and distribution as a function of electrochemical polarization applied at the electrode. Substantial improvement of reaction kinetics is found, consistent with previous reports [5]. In addition, we probe the effect of electrochemical and temperature conditions on the particle size, shape and distribution. In addition, we propose tuning the reducibility of parent oxides to be a good strategy in controlling the size and dispersion of the exsolved particles, and demonstrate this approach on epitaxial perovskite thin films. Moreover, our observations suggest oxygen vacancies to be the potential nucleation sites of the exsolved particles. The present study provides a new direction towards the generation of nanoparticle-size catalysts on the surface of perovskite oxides given the increasing demand for active and durable catalysts in the field of solid oxide cells and in other energy and fuels conversion processes. References: [1] G. Tsekouras et. al. Energy Environ. Sci., 2013, 6, 256–266 [2] Y. Sun et. al. J. Mater. Chem. A, 2015, 3, 11048–11056 [3] G. Dimitrakopoulos et. al. Sustainable Energy & Fuels 2019, 3, 2347-2355 [4] D. Neagu et. al. Nature Communications 8:1855 (2017) [5] J. Myung et. al. Nature 537 (2016) 528-531
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2020
    detail.hit.zdb_id: 2438749-6
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
  • 3
    Online Resource
    Online Resource
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-01, No. 36 ( 2020-05-01), p. 1470-1470
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-01, No. 36 ( 2020-05-01), p. 1470-1470
    Abstract: The global sustainability targets require technologies to provide clean chemical and fuel feedstock molecules on a large scale often by employing renewable electricity as the energy input. Nowadays, syngas (carbon monoxide and hydrogen), the key intermediate for synthetic fuels through Fischer-Tropsch, is primarily generated from fossil fuels, which are responsible for gigantic energy consumption and green-house gases emissions. The co-electrolysis of carbon dioxide and steam in solid oxide electrolysis cells (SOECs) constitutes an emerging route for syngas feedstock production and thus, for storing the intermittent renewable electricity in the form of chemical bonds 1 . In SOECs, the Ni-based cermets are the most commonly employed materials as fuel electrodes due to their high electro-catalytic activity. Ni-based cermets, however, exhibit significant drawbacks, such as Ni coarsening under redox conditions and coking in the electrochemical active zone during CO 2 electrolysis 3 . Perovskite oxides (ABO 3 ) are the most promising alternatives due to their exceptional redox stability, extensive range of functionalities and the concept of exsolution. During exsolution, metallic nanoparticles of reducible species (usually from the B-site) grow at the surface of the perovskite oxide scaffold at reducing atmospheres, i.e. hydrogen-rich gas phase 3 or imposition of high cathodic overpotentials 4 . Hence, perovskite oxide electrodes can be decorated with uniformly dispersed, anchored, coke and oxidation-resistant metal nanoparticles that can dramatically enhance the electrocatalytic performance and stability of the cell 4 . Compared to the slower exsolution via thermochemical reduction by hydrogen, the exsolution driven by electrochemical poling require only some minutes under high applied bias (~2.0 V) to form considerably higher population densities of metal nanoparticles on the oxide surface. Therefore, this method does not only offer, new pathways to electrode nanostructuring but also simplifies remarkably their preparation procedure 4 . Along these lines, here, we employ A-site deficient perovskites capable of exsolution, ((La,Ca)(Ti,M)O 3 (LCT-M, M = Ni, Fe, Rh), as fuel electrodes (cathode) in ZrO 2 -based electrolyte supported cells for the high temperature steam and/or carbon dioxide electrolysis process. To achieve nucleation of the metal nanoparticles, reduction by both hydrogen and bias is investigated. Additionally, the effect of the imposed overpotential and gas atmosphere on the population, nature and shape of the particles is explored and it is correlated to the apparent cell performance during electrolysis. References [1] Y. Zheng, J. Wang, B. Yu, W. Zhang, J. Chen, J. Qiao, J. Zhang, Chem. Soc. Rev. 46 (2017) 1427-1463. [2] J. T. S. Irvine, D. Neagu, M. C. Verbraeken, C. Chatzichristodoulou, C. Graves, M. B. Mogensen, Nat. Energy 2016, 1, 15014. [3] D. Neagu, G. Tsekouras, D.N, Miller, H. Menard, J.T.S. Irvine, Nat. Chem. 11 (2013) 916–923. [4] J. Myung, D. Neagu, D. N. Miller, J. T. S. Irvine, Nature 2016, 537, 528.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2020
    detail.hit.zdb_id: 2438749-6
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
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