LAUSR

Abstract Heteroatom doping of carbonaceous materials can effectively modulate their physiochemical properties, providing great potentials to design innovative architectures with enhanced performance for energy-related applications. Herein, we report a versatile molecular-based strategy for the in-situ synthesis of highly-ordered, heteroatom-doped mesoporous carbon frameworks (MCFs). Our approach is based on the transformation of self-assembled superlattices consisting of Fe3O4 nanocrystals (NCs) with desired surface-coating molecular species, which are realized by exploiting versatile surface chemistry of colloidal NCs. By this strategy, various heteroatoms, such as N, B, and S, can be directly incorporated into the simultaneously formed MCFs with a homogeneous distribution. Taking advantage of their highly ordered and interconnected mesoporosity, tunable doping level, and high surface area, such heteroatom-doped MCFs show great promise for energy-related applications. We show that the N-doped MCFs (N-MCFs) exhibit significantly enhanced catalytic activity relative to their undoped counterparts when evaluated as electrocatalyst for oxygen reduction reaction. Likewise, the N-MCFs can also be used as electrode material for constructing supercapacitors with outstanding cycling stability and rate performance. This work offers a surface chemistry approach for the direct synthesis of highly-ordered MCFs containing homogeneously distributed heteroatoms, which are suitable for applications in various energy conversion and storage devices.