The development of oxygen evolution reaction (OER) electrocatalysts remains a major challenge that requires significant advances in both mechanistic understanding and material design. Recent studies show that oxygen from the perovskite oxide lattice could participate in the OER via a lattice oxygen-mediated mechanism, providing possibilities for the development of alternative electrocatalysts that could overcome the scaling relations-induced limitations found in conventional catalysts utilizing the adsorbate evolution mechanism. Here we distinguish the extent to which the participation of lattice oxygen can contribute to the OER through the rational design of a model system of silicon-incorporated strontium cobaltite perovskite electrocatalysts with similar surface transition metal properties yet different oxygen diffusion rates. The as-derived silicon-incorporated perovskite exhibits a 12.8-fold increase in oxygen diffusivity, which matches well with the 10-fold improvement of intrinsic OER activity, suggesting that the observed activity increase is dominantly a result of the enhanced lattice oxygen participation.
22 November 2017 in Journal of Materials Chemistry A
Electrochemical reduction of gaseous feeds such as CO2, CO, and N2 holds promise for sustainable energy and chemical production. Practical application of this technology is impeded by slow mass transport of the sparingly soluble gases to conventional planar electrodes. Gas diffusion electrodes (GDEs) maintain a high gas concentration in the vicinity of the catalyst and improve mass transport, thereby resulting in current densities higher by orders of magnitude. However, gaseous feeds cause changes to the GDE environment, and specific features are required to efficiently tune the product selectivity and improve reaction stability. Herein, with a comprehensive review of the challenges and advances in GDE development for various electrocatalytic reactions, we intend to complement the body of material-focused reviews. This review outlines GDE fundamentals and highlights key advantages of GDE over conventional electrodes. Through critical discussion about steps in GDE fabrication, and specific shortcomings and remedial strategies for various electrochemical applications, this review discusses connections, unique design criteria, and potential opportunities for gas-fed reactions and desired products. Finally, priorities for future studies are suggested, to support the advancement and scale-up of GDE-based electrochemical technologies.