Towards the direct instrumental identification of active electrocatalytic sites using scanning tunneling microscopy

• Applicant: Professor Dr. Aliaksandr Bandarenka
• Subject Area: Physical Chemistry of Molecules, Liquids and Interfaces, Biophysical Chemistry
• Term: from 2016 to 2021
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 320825100

• Final Report Year: 2021

Final Report Abstract

The project aim was to understand complex objects of nature with the development of a new informative and affordable research methodology, namely noise analysis in electrochemical scanning tunneling microscopy (n-EC-STM). The project utilized the basic idea that under reaction conditions, the parameters defining the tunneling barrier over the catalytically active sites in contact with liquid electrolytes should be different, and, importantly, vary with time (e.g., due to approaching reactants and/or departing products), compared to those over the inactive sites. Therefore, the tunneling current measured between the tip and the sample under potential control should also change with time differently, revealing local processes. By comparing the tunneling current as a function of time and tip-to-surface distance over different surface sites, it was possible to elucidate the location of the catalytic centers for systems and reactions relevant for energy provision schemes. Those included the hydrogen evolution and oxygen reduction at various Ptbased and platinum-free catalytic surfaces. Our obtained results strongly support this initial basic idea on the n-EC-STM.

Publications

• Direct instrumental identification of catalytically active surface sites. Nature 549 (2017) 74–77
  J.H.K. Pfisterer, Y. Liang, O. Schneider, A.S. Bandarenka
  
• Engineering of highly active silver nanoparticles for oxygen electroreduction via simultaneous control over their shape and size. Advanced Sustainable Systems 1 (2017) 1700117
  B. Garlyyev, Y. Liang, F.K. Butt, A.S. Bandarenka
  
• Electrochemical scanning probe microscopies in electrocatalysis. Small Methods 3 (2019) 1800387
  Y. Liang, J.H.K. Pfisterer, D. Mclaughlin, C. Csoklich, L. Seidl, A.S. Bandarenka, O. Schneider
  
• In-situ visualization of hydrogen evolution sites on helium ion treated molybdenum dichalcogenides under reaction conditions. NPJ 2D Materials and Applications 3 (2019) 25
  E. Mitterreiter, Y. Liang, M. Golibrzuch, D. McLaughlin, C. Csoklich, J.D. Bartl, A. Holleitner, U. Wurstbauer, A.S. Bandarenka
  
• Revealing active sites for hydrogen evolution at Pt and Pd atomic layers on Au surfaces. ACS Applied Materials and Interfaces 11 (2019) 12476–12480
  Y. Liang, C. Csoklich, D. McLaughlin, O. Schneider, A.S. Bandarenka
  
• Revealing the nature of active sites in electrocatalysis. Chemical Science 10 (2019) 8060-8075
  B. Garlyyev, J. Fichtner, O. Piqué, O. Schneider, A.S. Bandarenka, F. Calle-Vallejo
  
• The nature of active centers catalyzing oxygen electro-reduction at platinum surfaces in alkaline media. Energy & Environmental Science 12 (2019) 351-357
  Y. Liang, D. Mclaughlin, C. Csoklich, O. Schneider, A.S. Bandarenka
  
• Theoretical and experimental identification of active electrocatalytic surface sites. Current Opinion in Electrochemistry 14 (2019) 206-21
  B. Garlyyev, Y. Liang, S. Xue, S. Watzele, J. Fichtner, W.J. Li, X. Ding, A.S. Bandarenka
  
• Enhancing the hydrogen evolution reaction activity of platinum electrodes in alkaline media using Ni-Fe clusters. Angewandte Chemie International Edition 59 (2020) 10934-10938
  S. Xue, R.W. Haid, R.M. Kluge, X. Ding, B. Garlyyev, J. Fichtner, S. Watzele, S. Hou, A.S. Bandarenka
  
• In-situ quantification of the local electrocatalytic activity via electrochemical scanning tunneling microscopy. Small Methods 4 (2020) 2000710
  R.W. Haid, R.M. Kluge, Y. Liang, A.S. Bandarenka