Freeze–Thaw‐Promoted Fabrication of Clean and Hierarchically Structured Noble‐Metal Aerogels for Electrocatalysis and Photoelectrocatalysis

Abstract Noble‐metal aerogels (NMAs) have drawn increasing attention because of their self‐supported conductive networks, high surface areas, and numerous optically/catalytically active sites, enabling their impressive performance in diverse fields. However, the fabrication methods suffer from tedious procedures, long preparation times, unavoidable impurities, and uncontrolled multiscale structures, discouraging their developments. By utilizing the self‐healing properties of noble‐metal aggregates, the freezing‐promoted salting‐out behavior, and the ice‐templating effect, a freeze–thaw method is crafted that is capable of preparing various hierarchically structured noble‐metal gels within one day without extra additives. In light of their cleanliness, the multi‐scale structures, and combined catalytic/optical properties, the electrocatalytic and photoelectrocatalytic performance of NMAs are demonstrated, which surpasses that of commercial noble‐metal catalysts.