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Publications (21/21 displayed)

  • 2024Cation effects on the acidic oxygen reduction reaction at carbon surfacescitations
  • 2024Controllable Si oxidation mediated by annealing temperature and atmospherecitations
  • 2024Meta-kinks are key to binder performance of poly(arylene piperidinium) ionomers for alkaline membrane water electrolysis using non-noble metal catalysts5citations
  • 2024Synthetic design of active and stable bimetallic PtTi nanoparticle electrocatalysts for efficient oxygen reduction at fuel cell cathodescitations
  • 2024Integration of Multijunction Absorbers and Catalysts for Efficient Solar‐Driven Artificial Leaf Structures: A Physical and Materials Science Perspective6citations
  • 2023A Life-Cycle of Ni in Proton Exchange Membrane Fuel Cellscitations
  • 2022Metallic Iridium Thin-Films as Model Catalysts for the Electrochemical Oxygen Evolution Reaction (OER)—Morphology and Activitycitations
  • 2022Low‐Pt NiNC‐Supported PtNi Nanoalloy Oxygen Reduction Reaction Electrocatalysts—In Situ Tracking of the Atomic Alloying Processcitations
  • 2022High Power Density Automotive Membrane Electrode Assembliescitations
  • 2022Controllable Si oxidation mediated by annealing temperature and atmosphere3citations
  • 2022Ir-Ni Bimetallic OER Catalysts Prepared by Controlled Ni Electrodeposition on Irpoly and Ir(111)citations
  • 2020P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction375citations
  • 2019Real-time imaging of activation and degradation of carbon supported octahedral Pt–Ni alloy fuel cell catalysts at the nanoscale using in situ electrochemical liquid cell STEMcitations
  • 2018A comparison of rotating disc electrode, floating electrode technique and membrane electrode assembly measurements for catalyst testing109citations
  • 2018Polyformamidine-Derived Non-Noble Metal Electrocatalysts for Efficient Oxygen Reduction Reaction58citations
  • 2017Record activity and stability of dealloyed bimetallic catalysts for proton exchange membrane fuel cellscitations
  • 2017From molecular copper complexes to composite electrocatalytic materials for selective reduction of CO2 to formic acidcitations
  • 2016IrOx core-shell nanocatalysts for cost- and energy-efficient electrochemical water splittingcitations
  • 2015Hydrophobic Nanoreactor Soft-Templating: A Supramolecular Approach to Yolk@Shell Materials41citations
  • 2015Reversible amorphization and the catalytically active state of crystalline Co3O4 during oxygen evolutioncitations
  • 2015From molecular copper complexes to composite electrocatalytic materials for selective reduction of CO2 to formic acid73citations

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Co-Authors (by relevance)

  • Paul, Benjamin
  • Knop-Gericke, Axel
  • Sharapa, Dmitry I.
  • Behrens, Silke
  • Studt, Felix
  • Teschner, Detre
  • Hubner, Jessica L.
  • Kang, Jiaqi
  • Siahrostami, Samira
  • Nong, Hong Nhan
  • Kroschel, Matthias
  • Lucchetti, Lanna E. B.
  • Wang, Honglei
  • Schaaf, Peter
  • Klingenhof, Malte
  • Flock, Dominik
  • Wang, Dong
  • Li, Feitao
  • Metzler, Lukas
  • Sommer, Michael
  • Koch, Susanne
  • Vierrath, Severin
  • Merzdorf, Thomas
  • Weber, Richard
  • Meier-Haack, Jochen
  • Lu, Jiasheng
  • Herzog, Antonia
  • Selve, Sören
  • Schmidt, Johannes
  • Amitrano, Raffaele
  • Kühl, Stefanie
  • Dionigi, Fabio
  • Bergmann, Arno
  • Roldan Cuenya, Beatriz
  • Bonastre, Alejandro M.
  • Chattot, Raphaël
  • Gutierrez, Martha Briceno De
  • Drnec, Jakub
  • Ronovský, Michal
  • Fusek, Lukáš
  • Pan, Lujin
  • Mirolo, Marta
  • Hrbek, Tomas
  • Brooke, Emily
  • Kubát, Jan
  • Götz, Daniel
  • Polani, Shlomi
  • Myllymäki, Mila
  • Kúš, Peter
  • Dunseath, Olivia
  • Sharman, Jonathan
  • Martens, Isaac
  • Bernitzky, Cornelius
  • Spöri, Camillo
  • Pawolek, Zarina
  • Nong, Hong
  • Özer, Ebru
  • Feng, Quanchen
  • Heggen, Marc
  • Wang, Xingli
  • Weber, Konstantin
  • Hodgkinson, Adam
  • Buche, Silvain
  • Spackova, Martina
  • Nesling, Emily
  • Gasteiger, Hubert A.
  • Albert, Albert
  • Brimaud, Sylvain
  • Zink, Stefan
  • Finkenwirth, Olav
  • Loichet, Paulette A.
  • Ponomarev, Ivan
  • Muggli, Mark
  • Barsch, Hannes
  • Joerissen, Ludwig
  • Rozière, Jacques
  • Cavaliere, Sara
  • Zaton, Marta
  • Jones, Deborah J.
  • Araujo, Jorge
  • Kropp, Thomas
  • Mavrikakis, Manos
  • Mayrhofer, Karl
  • Sinev, Ilya
  • Mingers, Andrea
  • Cullen, David
  • Silvioli, Luca
  • Jaouen, Frédéric
  • Rossmeisl, Jan
  • Oguz, Ismail Can
  • Luo, Fang
  • Wen, Ju
  • Wagner, Stephan
  • Sougrati, Moulay Tahar
  • Mineva, Tzonka
  • Kramm, Ulrike
  • Zitolo, Andrea
  • Roy, Aaron
  • De Araujo, Jorge Ferreira
  • Muller, David A.
  • Padgett, Elliot
  • Beermann, Vera
  • Holtz, Megan E.
  • Martinez Bonastre, Alejandro
  • Schneider, Oliver
  • Hawkins, Alex
  • Seidl, Lukas
  • Knoll, Alois, C.
  • Ercolano, Giorgio
  • Sladjana, Martens
  • Asen, Ludwig
  • Martens, Sladjana
  • Zalitis, Chris
  • Jones, Deborah
  • Sharman, Jonathan, D. B.
  • Fischer, Anna
  • Melke, Julia
  • Sahraie, Nastaran Ranjbar
  • Pardo Pérez, Laura C.
  • Huang, Xing
  • Elsässer, Patrick
  • Enthaler, Stephan
  • White, Robin J.
  • Kraehnert, Ralph
  • Theobald, Brian R.
  • Shao-Horn, Yang
  • Gan, Lin
  • Carlton, Christopher E.
  • Kongkanand, Anusorn
  • Kukreja, Ratandeep S.
  • Han, Binghong
  • Omalley, Rachel
  • Wagner, Frederick T.
  • Andreiadis, Eugen S.
  • Huan, Tran Ngoc
  • Royal, Guy
  • Cobo, Saioa
  • Dau, Holger
  • Heidkamp, Jonathan
  • Simon, Philippe
  • Fontecave, Marc
  • Artero, Vincent
  • Derat, Etienne
  • Willinger, Elena
  • Guiet, Amandine
  • Driess, Matthias
  • Polte, Jörg
  • Göbel, Caren
  • Vainio, Ulla
  • Zaharieva, Ivelina, H.
  • Klingan, Katharina
  • Schlaad, Helmut
  • Lublow, Michael
  • Reier, Tobias, R.
  • Ferreira De Araújo, Jorge
  • Reier, Tobias
  • Martínez Moreno, Elías
  • Gliech, Manuel
  • Chernev, Petko
  • Andreiadis, Eugen. S.
OrganizationsLocationPeople

document

A Life-Cycle of Ni in Proton Exchange Membrane Fuel Cells

  • Bonastre, Alejandro M.
  • Chattot, Raphaël
  • Gutierrez, Martha Briceno De
  • Drnec, Jakub
  • Ronovský, Michal
  • Fusek, Lukáš
  • Dionigi, Fabio
  • Pan, Lujin
  • Mirolo, Marta
  • Hrbek, Tomas
  • Klingenhof, Malte
  • Strasser, Peter
  • Brooke, Emily
  • Kubát, Jan
  • Götz, Daniel
  • Polani, Shlomi
  • Myllymäki, Mila
  • Kúš, Peter
  • Dunseath, Olivia
  • Sharman, Jonathan
  • Martens, Isaac
Abstract

<jats:p>The usage of Proton Exchange Membrane Fuel Cells (PEMFCs) in the automotive industry is currently limited by the price, performance, and durability of a platinum catalyst. Alloying with nickel provides lower cost and enhances activity. However, the membrane electrode assembly (MEA) performance is, in practice, much lower than expected from liquid laboratory experiments on the catalyst layer. One of the identified issues is Ni leaching from nanoparticles (NPs) and subsequent Ni poisoning of the Nafion membrane.</jats:p><jats:p>Here, we use Wide-Angle X-ray Scattering (WAXS) and X-ray Absorption Near-Edge Structure (XANES) to follow Ni dissolution from the catalyst layer and its movement in the MEA. We shine (synchrotron) light on the full life cycle of Ni, starting from (i) characterization of the catalyst powder, followed by (ii) the changes in catalyst composition during the ink-making process and (iii) membrane coating and finishing with (iv) NP characterization and Ni tracking during the operation of MEAs.</jats:p><jats:p>Proper incorporation of PtNi catalyst requires modification of all the aforementioned steps that are otherwise well optimized for pure Pt catalyst. It is even more critical for shape-controlled octahedra (oh) PtNi NPs as their activity is closely related to their structure [1]. Highly active oh-PtNi NPs are usually made from precursors such as Nickel(II) bis(acetylacetonate). Using EDX, we find precursor residues in catalyst powders that dissolve upon further processing and add to membrane poisoning. We conclude that we need to develop a cleaning protocol that would remove all Ni residue while retaining the nanoparticle shape.</jats:p><jats:p>During ink-making, high ionomer concentrations and elevated temperatures promote Ni dissolution from the catalyst, which can, in turn, poison the membrane even before the MEA is put in use. With the WAXS technique, we track the dissolution during ink-making and MEA operation by following changes in lattice parameter, showing the dynamics and the extent of Ni dissolution in each step of aging.</jats:p><jats:p>Furthermore, we use angle-resolved XANES to track the movement of dissolved Ni. We show that Ni ions are getting reduced back to metallic form within the MEA, likely due to hydrogen crossover. The presence of such a metal band in the membrane blocks proton conductivity and decreases performance [2]. That is why it is crucial to set manufacturing and operational boundaries to prevent dissolution.</jats:p><jats:p>For this reason, we follow WAXS total scattering intensity during oxidation and reduction cycles to understand the Ni dissolution dynamics during operation. We find that limiting both upper and lower potential cycling limits greatly reduces the redox extent and subsequent dissolution. It is, therefore, possible to find and understand the trade-off between high power density and dissolution in operational cells.</jats:p><jats:p>Even though this work looks at the Ni life cycle, the presented techniques and conclusions are transferable to all multimetallic high-performance PEMFC catalysts.</jats:p><jats:p>References:</jats:p><jats:p>[1] Shlomi Polani et al. ACS Appl. Mater. Interfaces 2022, 14, 26, 29690–29702</jats:p><jats:p>[2] Wu Bi et al. Electrochem. Solid-State Lett. 2007 10 B101</jats:p><jats:p><jats:inline-formula><jats:inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="2277fig1.jpg" xlink:type="simple" /></jats:inline-formula></jats:p><jats:p>Figure 1</jats:p><jats:p />

Topics
  • nanoparticle
  • density
  • impedance spectroscopy
  • nickel
  • experiment
  • Platinum
  • Hydrogen
  • leaching
  • aging
  • Energy-dispersive X-ray spectroscopy
  • wide-angle X-ray scattering
  • aging