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

Year: 2025

Type: article

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 hydrogen evolution reaction.

Source: RSC Applied Interfaces

DOI: 10.1039/d5lf00064e

Authors: Mi Yeon Byun, Lili Liu, Daniel Mejía-Rodríguez, Eric D. Walter, Zihua Zhu, Niri Govind, Tom Autrey, Maria L. Sushko

Institution: Pacific Northwest National Laboratory

Language: English

Topic: Electrocatalysts for Energy Conversion

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

Open Access status: diamond

Funders: U.S. Department of Energy, Battelle, National Energy Research Scientific Computing Center, Office of Science, Basic Energy Sciences, Biological and Environmental Research, Pacific Northwest National Laboratory, Division of Materials Sciences and Engineering

OpenAlex ID: W4411216988