Nucleobases-derived carbon materials: Synthesis and application in heterogeneous catalysis

Natural nitrogen-heterocycles biomolecules have been widely used in the construction of supramolecular selfassemblies due to their abundant resources and multiple interaction sites, such as hydrogen bonding, pi-pi stacking, van der Waals forces. Herein, we propose a quite innovative strategy to produce two-dimensional (2D) carbon materials by direct pyrolysis of various nucleobases (e.g. guanine, adenine, uracil, cytosine xanthine, and hypoxanthine). These nucleobases can pre-organize a planar network structure through hydrogen bonding interaction. The multiple hydrogen-bonding can be stable at relatively high temperature, which limits C-C or C-N cleavage and formation in a 2D space. These 2D carbons show desirable features with highly sp2-conjugation, tunable heteroatom contents, and ultrathin thickness, without the need of any template or additional purification. Meanwhile, differences in internal structure allow easy control of the morphology of 2D carbons, porosity and surface chemical functionality at the molecular level. Moreover, the as-synthesized 2D carbons display very promising electrocatalytic ORR performance and catalytic performance for selective oxidization of ethylbenzene. Given the diversity in the structure of the nucleobase moiety, they represent ideal building blocks for the catalyst-free and metal-free formation of 2D carbon architectures.

Automated summary

This study proposes an innovative method for preparing two-dimensional carbon materials by directly pyrolyzing various nucleobases. These 2D carbons exhibit desirable features, including highly conjugated sp2 structure, tunable heteroatom contents, and ultrathin thickness, without the need for any template or additional purification. Additionally, these 2D carbons also show excellent electrocatalytic and catalytic performance.