Controlling N speciation in solution synthesis of N-doped carbon materials

Abstract

Carbon-based materials, such as graphite and its functionalized/doped derivatives, are promising lightweight layered materials for hydrogen activation and storage. Their propensity to control the thermodynamics of hydrogen binding and the kinetics of hydrogen mobility strongly depends on the speciation and the arrangement of dopants. In this study, we demonstrate precise control over dopant speciation and clustering in nitrogen-containing layered carbon materials during hydrothermal synthesis. Through extensive spectroscopic characterization and first principles simulations, we demonstrate that the formation of N-motifs can be controlled by the choice of precursor and synthesis temperature. The distinct three-dimensional architecture and porosity in graphene oxide and carbon nitride-derived materials furnish a synthetic pathway for precise control over the local and global structure of nitrogen-doped carbon materials and their activity toward the activation of molecular hydrogen.

Graphical abstract: Controlling N speciation in solution synthesis of N-doped carbon materials

Supplementary files

Article information

Article type
Paper
Submitted
04 Mar 2025
Accepted
08 Jun 2025
First published
11 Jun 2025
This article is Open Access
Creative Commons BY-NC license

RSC Appl. Interfaces, 2025, Advance Article

Controlling N speciation in solution synthesis of N-doped carbon materials

M. Y. Byun, L. Liu, D. Mejía-Rodríguez, E. D. Walter, Z. Zhu, N. Govind, T. Autrey and M. L. Sushko, RSC Appl. Interfaces, 2025, Advance Article , DOI: 10.1039/D5LF00064E

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