Three-Dimensional Porous Indium Single-Atom Catalysts with Improved Accessibility for CO2 Reduction to Formate

Single-atom catalysts (SACs) present substantial potential in electrocatalytic CO2 reduction reactions; however, inferior accessibility of single-atom sites to CO2 limits the overall CO2RR performances. Herein, we propose to improve the accessibility between In sites and CO2 through the construction of a three-dimensional (3D) porous indium single-atom catalyst (In1/NC-3D). The NaCl template-mediated synthesis strategy generates the unique 3D porous nanostructure of In1/NC-3D. Multiple characterizations validate that In1/NC-3D exhibits increased exposure of active sites and enhanced CO2 transport/adsorption capacity compared to the bulk In1/NC, thus improving accessibility of active sites to CO2. As a result, the In1/NC-3D presents superior CO2RR performance to the bulk In1/NC, with a partial current density of formate of 67.24 mA cm–2 at −1.41 V, relative to a reversible hydrogen electrode (vs RHE). The CO2RR performances with high formate selectivity at a large current density also outperform most reported In-based SACs. Importantly, the In1/NC-3D is demonstrated to maintain an FEformate of >82% at −66.83 mA·cm–2 over 21 h. This work highlights the design of a 3D porous single-atom catalyst for efficient CO2RR, promoting the development of advanced catalysts toward advanced energy conversion.