A Systems Approach to Resolving the Valence Electronic Structures in Carbon Nitrides

Nnamdi C. Okey; Aditi Bhattacherjee

doi:10.1021/acs.jpcc.5c03260

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A Systems Approach to Resolving the Valence Electronic Structures in Carbon Nitrides

Journal article

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Peer reviewed

A Systems Approach to Resolving the Valence Electronic Structures in Carbon Nitrides

Nnamdi C. Okey and Aditi Bhattacherjee

Journal of physical chemistry. C, Vol.129(29), pp.13488-13496

07/16/2025

DOI: 10.1021/acs.jpcc.5c03260

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Abstract

The controlled polymerization of common organic precursor molecules at high temperatures is known to produce carbon nitride oligomers and polymers with a wide range of photocatalytic activity. However, tracking the electronic structures precisely in these complex functional systems remains a significant challenge. Here, we utilize bottom-up and top-down methods of high-temperature polymerization and solution-phase exfoliation to directly reveal the frontier molecular orbitals that give rise to near- and above-band edge transitions. Aqueous dispersions of the oligomeric fractions manifest a progressive increase in a molecular exciton of mixed ππ*/nπ* character that is reproducible with multiple precursors and tractable using theory. The results offer new electronic structural insights and outline a systems approach to resolving the structure-dependent optoelectronic properties of photocatalytic carbon nitrides.

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Diffraction

Inorganic Carbon Compounds

Melamine

Oligomers

Precursors

Details

Title: Subtitle: A Systems Approach to Resolving the Valence Electronic Structures in Carbon Nitrides
Creators: Nnamdi C. Okey - University of Iowa
Aditi Bhattacherjee - University of Iowa
Resource Type: Journal article
Publication Details: Journal of physical chemistry. C, Vol.129(29), pp.13488-13496
DOI: 10.1021/acs.jpcc.5c03260
ISSN: 1932-7447
eISSN: 1932-7455
Publisher: American Chemical Society
Number of pages: 9
Grant note: American Chemical Society Petroleum Research Fund: 66711-DNI6 ACS Petroleum Research Fund under Doctoral New Investigator Grant: 66711-DNI6 ACS PRF
This work was supported by the donors of ACS Petroleum Research Fund under Doctoral New Investigator Grant 66711-DNI6. A.B. served as Principal Investigator on ACS PRF 66711-DNI6 that provided support for N.C.O. This research was supported in part through computational resources (University of Iowa), shared instrument facilities (Department of Chemistry, University of Iowa), Materials Analysis, Testing, and Fabrication (MATFab) Facility (University of Iowa), and instructional laboratories (Department of Chemistry, University of Iowa).
Language: English
Date published: 07/16/2025
Academic Unit: Chemistry
Record Identifier: 9984865439802771

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