Optimization of electrocatalysts for fuel cell applications without alloying: a joint theoretical and experimental study

• Applicants: Professor Dr. Aliaksandr Bandarenka; Professor Dr.-Ing. Alessio Gagliardi
• Subject Area: Physical Chemistry of Solids and Surfaces, Material Characterisation ; Experimental Condensed Matter Physics
• Term: from 2017 to 2021
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 355784621

• Final Report Year: 2021

Final Report Abstract

The project aim was to use recent experimental discoveries and a fundamental understanding of how one can increase the surface activity of pure Pt by at least the factor of 3.5-5 without any alloying to design active and more stable electrocatalysts for the oxygen reduction reaction. The key fact in this approach is that it is possible to increase the activity of, e.g., Pt by controlling the atom coordination near the ORR active sites. The particular aim was to elucidate and implement optimized structures with the maximum density of active sites of right coordination, improved stability, and local mass transport properties. Successful realization of the proposed project would not only clearly demonstrate the researchers and engineers how to improve the existing materials even without alloying; it would likely establish an entirely new methodology for the development of heterogeneous electrocatalysts based on a combination of theoretical calculations of different levels and experimental approaches which elaborate open nanostructured materials applicable in the “real-world” electrocatalysis.

Publications

• Optimizing the size of platinum nanoparticles for enhanced oxygen electro-reduction mass activity. Angewandte Chemie International Edition (2019) 9596-9600
  B. Garlyyev, K. Kratzl, M. Rück, J. Michalička, J. Fichtner, J. Macak, T. Kratky, S. Günther, M. Cokoja, A.S. Bandarenka, A. Gagliardi, R. Fischer
  (See online at https://doi.org/10.1002/anie.201904492)
• Revealing the nature of active sites in electrocatalysis. Chemical Science (2019) 8060-8075
  B. Garlyyev, J. Fichtner, O. Piqué, O. Schneider, A.S. Bandarenka, F. Calle-Vallejo
  (See online at https://doi.org/10.1039/c9sc02654a)
• The nature of active centers catalyzing oxygen electro-reduction at platinum surfaces in alkaline media. Energy & Environmental Science (2019) 351-357
  Y. Liang, D. Mclaughlin, C. Csoklich, O. Schneider, A.S. Bandarenka
  (See online at https://doi.org/10.1039/c8ee03228a)
• Advanced bifunctional oxygen reduction and evolution electrocatalyst derived from surface-mounted metal-organic frameworks. Angewandte Chemie International Edition (2020) 5837-5843
  W.-J. Li, S. Xue, S. Watzele, S. Hou, J. Fichtner, A.L. Semrau, L. Zhou, A. Welle, A.S. Bandarenka, R.A. Fischer
  (See online at https://doi.org/10.1002/anie.201916507)
• Electrochemical top-down synthesis of C-supported Pt nanoparticles with controllable shape and size: mechanistic insights and application. Nano Research (2020)
  B. Garlyyev, S. Watzele, J. Fichtner, J. Michalička, A. Schökel, A. Senyshyn, A. Perego, D. Pan, H. El-Sayed, J.M. Macak, P. Atanassov, I.V. Zenyuk, A.S. Bandarenka
  (See online at https://doi.org/10.1007/s12274-020-3281-z)
• Enhancing the hydrogen evolution reaction activity of platinum electrodes in alkaline media using Ni-Fe clusters. Angewandte Chemie International Edition (2020) 10934-10938
  S. Xue, R.W. Haid, R.M. Kluge, X. Ding, B. Garlyyev, J. Fichtner, S. Watzele, S. Hou, A.S. Bandarenka
  (See online at https://doi.org/10.1002/anie.202000383)
• In-situ quantification of the local electrocatalytic activity via electrochemical scanning tunneling microscopy. Small Methods (2020) 2000710
  R.W. Haid, R.M. Kluge, Y. Liang, A.S. Bandarenka
  (See online at https://doi.org/10.1002/smtd.202000710)
• Tailoring the oxygen reduction activity of Pt nanoparticles through surface defects: a simple top-down approach. ACS Catalysis (2020) 3131-3142
  J. Fichtner, S. Watzele, B. Garlyyev, R. Kluge, F. Haimerl, H. El-Sayed, W.-J. Li, F. Maillard, L. Dubau, R. Chattot, J. Michalicka, J. Macak, W. Wang, D. Wang, T. Gigl, C. Hugenschmidt, A.S. Bandarenka
  (See online at https://doi.org/10.1021/acscatal.9b04974)
• Temperature effects in polymer electrolyte membrane fuel cells. ChemElectroChem (2020) 3545-3568
  T. Lochner, R.M. Kluge, J. Fichtner, H.A. El-Sayed, B. Garlyyev, A.S. Bandarenka
  (See online at https://doi.org/10.1002/celc.202000588)
• In-situ detection of active sites for carbon-based bifunctional oxygen reduction and evolution catalysis. Electrochimica Acta (2021) 138285
  R.W. Haid, R.M. Klug, T.O. Schmidt, A.S. Bandarenka
  (See online at https://doi.org/10.1016/j.electacta.2021.138285)