Item

Abstract

The combination of operando and computational X-ray spectroscopies has shown promise for building accurate models of active catalyst surfaces. Operando spectroscopy captures metastable active surfaces and computational spectroscopy uses this information to aid in building models for first principles reaction simulations. Herein, we review recent efforts and outline future opportunities to study the oxygen evolution reaction (OER) by combining operando spectroscopies and first principles modeling. We begin by showcasing how explicit simulation of operando-collected spectra has helped validate an OER mechanism over Ir-based catalysts involving electron-deficient oxygen, or O^I−. We continue by reviewing efforts on 3d transition metal (TM) oxyhydroxides, where operando studies again suggest O^I− is critical. While for these materials, changes in O^I− coverage have been argued to cause qualitative mechanistic differences, comparative operando and computational spectroscopic studies are still lacking. We close by outlining how such comparative studies would aid in testing mechanistic claims on 3d TM oxyhydroxides.