Work

Graphite-Supported Pt n Cluster Electrocatalysts: Major Change of Active Sites as a Function of the Applied Potential

Year: 2022

Type: article

Abstract: The oxygen reduction reaction (ORR) plays a key role in renewable energy transformation processes. Unfortunately, it is inherently sluggish, which greatly limits its industrial application. Sub-nano-cluster-decorated electrode interfaces are promising candidate ORR electrocatalysts. However, understanding the nature of the active sites on these catalysts under electrocatalytic conditions presents a formidable challenge for both experiment and theory, due to their dynamic fluxional character. Here, we combine global optimization with the electronic Grand Canonical DFT to elucidate the structure and dynamics of subnano Pt n clusters deposited on electrified graphite. We show that, under electrochemical conditions, these clusters exist as statistical ensembles of multiple states, whose fluxionality is greatly affected by the applied potential, electrolyte, and adsorbate coverage. The results reveal the presence of potential-dependent active sites and, hence, reaction energetics.

Source: ACS Catalysis

DOI: 10.1021/acscatal.2c04643

Authors: Julen Munarriz, Zisheng Zhang, Philippe Sautet, Anastassia N. Alexandrova

Institutions: University of California, Los Angeles, Universidad de Oviedo, California NanoSystems Institute

Language: English

Topic: Electrocatalysts for Energy Conversion

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: green

Funders: U.S. Department of Energy, National Energy Research Scientific Computing Center, Basic Energy Sciences