Multifunctional electroactive heteroatom-doped carbon aerogels

Abstract

The design and synthesis of highly active, durable, and cheap nanomaterials for various renewable energy storage and conversion applications is extremely desirable but remains challenging. Here, a green and efficient strategy to produce CoOx nanoparticles and surface N-co-doped carbon aerogels (Co-N-CAs) is reported by multicomponent surface self-assembly of commercially melamine sponge (CMS). In the methodology, the CMS simultaneously function as green N precursor for surface N doping and 3D support. The resulting Co-N-CAs exhibit 3D hierarchical, interconnected macro- and bimodal meso-porosity (6.3 nm and <4 nm), high surface area (1383 m(2) g(-1)), and highly dispersed, semi-exposured CoOx nanoparticles (diameter of 12.5 nm). The surface doping of N, semi-exposured configuration of CoOx nanoparticles and the penetrated complementary pores (<4 nm) in the carbon walls provide highly accessibility between electroactive components and electrolytes to improve reactivity. With their tailored architecture, the Co-N-CAs show superior electrocatalytic oxygen reduction (ORR) activities comparable to the commercially Pt/C catalysts, high specific capacitance (433 F g(-1)), excellent lithium storage (938 mAh g(-1)), and outstanding durability, making them very promising for advanced energy conversion and storage. In addition, the presented strategy can be extended to fabricate other metal oxide- and N-co-doped carbon aerogels for diverse energy-related applications.

Keywords: carbon aerogels; heteroatoms; lithium storage; oxygen reduction; supercapacitors.