Relationships between Atomic Level Surface Structure and Stability/Activity of Platinum Surface Atoms in Aqueous Environments

Lopes, Pietro P.; Strmcnik, Dusan; Tripkovic, Dusan; Connell, Justin G.; Stamenkovic, Vojislav; Markovic, Nenad M.

doi:10.1021/acscatal.5b02920

Title: Relationships between Atomic Level Surface Structure and Stability/Activity of Platinum Surface Atoms in Aqueous Environments

Journal Article · Mon Mar 07 00:00:00 EST 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b02920· OSTI ID:1352658

Lopes, Pietro P. ^[1]; Strmcnik, Dusan ^[1]; Tripkovic, Dusan ^[1]; Connell, Justin G. ^[1]; Stamenkovic, Vojislav ^[1]; Markovic, Nenad M. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

The development of alternative energy systems for clean production, storage and conversion of energy is strongly dependent on our ability to understand, at atomic-molecular-levels, functional links between activity and stability of electrochemical interfaces. Whereas structure-activity relationships are rapidly evolving, the corresponding structure-stability relationships are still missing. Primarily, this is because there is no adequate experimental approach capable of monitoring in situ stability of well-defined single crystals. Here, by blending the power of Inductively Coupled Plasma-Mass Spectrometer (ICP-MS) connected to a stationary probe to measure in situ and real time dissolution rates of surface atoms (at above 0.4 pg cm-2s-1 levels) and a rotating disk electrode method for monitoring simultaneously the kinetic rates of electrochemical reactions in a single unite, it was possible to establish almost “atom-by-atom” the structure-stability-activity relationships for platinum single crystals in both acidic and alkaline environments. Furthermore, we found that the degree of stability is strongly dependent on the coordination of surface atoms (less coordinated yields less stable), the nature of covalent (adsorption of hydroxyl, oxygen atoms and halides species), and non-covalent interactions (interactions between hydrated Li cations and surface oxide), the thermodynamic driving force for Pt complexation (Pt ion speciation in solution) and the nature of the electrochemical reaction (the oxygen reduction/evolution and CO oxidation reactions). Consequently, these findings are opening new opportunities for elucidating key fundamental descriptors that govern both activity and stability trends, that ultimately, will assist to develop real energy conversion and storage systems.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1352658

Journal Information:: ACS Catalysis, Vol. 6, Issue 4; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 160 works

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