One-Pot Synthesis of Hierarchically Macro- and Mesoporous Carbon Materials with Graded Porosity

Hierarchically porous materials are becoming increasingly important in catalysis, separation, and energy applications due to their advantageous diffusion and flux properties. Here we present the synthesis of hierarchically macro- and mesoporous carbon materials with graded porosity from a one-pot fabrication route. Organic–polymeric hybrids of a carbon precursor and poly­(isoprene)-<i>block</i>-poly­(styrene)-<i>block</i>-poly­(4-vinylpyridine) with graded porosity are obtained via coassembly and nonsolvent-induced phase separation. The membranes were carbonized at temperatures as high as 1100 °C with simultaneous decomposition of the block copolymer. The carbon materials show an open nanoporous top surface with narrow pore-size distribution that opens up into a graded macroporous support with increasing macropore size along the film normal and mesoporous walls, providing for highly accessible porosity with a large surface area of over 500 m² g^–1. Further, we expand the direct synthesis process to form well-dispersed metal nanoparticles (such as nickel and platinum) on the graded, hierarchically porous carbon materials. Our one-pot synthesis offers a facile approach to graded macro- and mesoporous carbons