Homologous Temperature Regulated Hierarchical Nanoporous Structures by Dealloying

Abstract Nanoporous metals, fabricated via dealloying, offer versatile applications but are typically limited to unimodal porous structures, which hinders the integration of conflicting pore‐size‐dependent properties. A strategy is presented that exploits the homologous temperature ( T H )‐dependent scaling of feature sizes to generate hierarchical porous structures through multistep dealloying at varied T H levels, adjusted by altering dealloying temperatures or the material melting points. This technique facilitates the creation of monolithic architectures of bimodal porous nickel and trimodal porous carbon, each characterized by well‐defined, self‐similar bicontinuous porosities across distinct length scales. These materials merge extensive surface area with efficient mass transport, showing improved current delivery and rate capabilities as electrodes in electrocatalytic hydrogen production and electrochemical supercapacitors. These results highlight T H as a unifying parameter for precisely tailoring feature sizes of dealloyed nanoporous materials, opening avenues for developing materials with hierarchical structures that enable novel functionalities.