Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts

Allison St. John; Hannah Flayhart; Shuting Xiang; Qian Qian; N. Aaron Deskins; Anatoly I. Frenkel; Jonathan Rochford; Gonghu Li

doi:10.1021/acsaom.5c00019

Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts

Allison St. John
, Hannah Flayhart
, Shuting Xiang
, Qian Qian
, N. Aaron Deskins
, Anatoly I. Frenkel
, Jonathan Rochford
, Gonghu Li

Chemistry

University of New Hampshire
University of Massachusetts Boston
Stony Brook University
Worcester Polytechnic Institute
United States Department of Energy

Research output: Contribution to journal › Article › peer-review

Abstract

Graphitic carbon nitride (C₃N₄) has been widely explored as a photoactive support for single-atom catalysts (SACs). In this study, three different π-rich aromatic dianhydrides are employed to introduce molecularly quantized trap states into the conduction band of C₃N₄ to facilitate efficient charge separation, and to promote an enhanced photocatalytic CO₂ reduction response. These modified C₃N₄ materials have been characterized structurally and spectroscopically for use as a support for Co-based SACs. In photocatalytic CO₂ reduction studies, the Co SAC on naphthalene dianhydride-doped C₃N₄ exhibited the highest activity and selectivity toward CO production among the Co SACs tested in this work. The observed improvement in photocatalytic CO₂-to-CO conversion activity correlates with trends in photoinduced charge separation, as revealed by photoluminescence spectroscopy.

Original language	English
Pages (from-to)	881-888
Number of pages	8
Journal	ACS Applied Optical Materials
Volume	3
Issue number	4
DOIs	https://doi.org/10.1021/acsaom.5c00019
State	Published - Apr 25 2025

ASJC Scopus Subject Areas

Spectroscopy
Electronic, Optical and Magnetic Materials
Atomic and Molecular Physics, and Optics

Keywords

carbon nitride
CO reduction
cobalt
photocatalysis
single-atom catalyst

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10.1021/acsaom.5c00019

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title = "Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts",

abstract = "Graphitic carbon nitride (C3N4) has been widely explored as a photoactive support for single-atom catalysts (SACs). In this study, three different π-rich aromatic dianhydrides are employed to introduce molecularly quantized trap states into the conduction band of C3N4 to facilitate efficient charge separation, and to promote an enhanced photocatalytic CO2 reduction response. These modified C3N4 materials have been characterized structurally and spectroscopically for use as a support for Co-based SACs. In photocatalytic CO2 reduction studies, the Co SAC on naphthalene dianhydride-doped C3N4 exhibited the highest activity and selectivity toward CO production among the Co SACs tested in this work. The observed improvement in photocatalytic CO2-to-CO conversion activity correlates with trends in photoinduced charge separation, as revealed by photoluminescence spectroscopy.",

keywords = "carbon nitride, CO reduction, cobalt, photocatalysis, single-atom catalyst",

author = "\{St. John\}, Allison and Hannah Flayhart and Shuting Xiang and Qian Qian and Deskins, \{N. Aaron\} and Frenkel, \{Anatoly I.\} and Jonathan Rochford and Gonghu Li",

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year = "2025",

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doi = "10.1021/acsaom.5c00019",

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T1 - Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts

AU - St. John, Allison

AU - Flayhart, Hannah

AU - Xiang, Shuting

AU - Qian, Qian

AU - Deskins, N. Aaron

AU - Frenkel, Anatoly I.

AU - Rochford, Jonathan

AU - Li, Gonghu

PY - 2025/4/25

Y1 - 2025/4/25

N2 - Graphitic carbon nitride (C3N4) has been widely explored as a photoactive support for single-atom catalysts (SACs). In this study, three different π-rich aromatic dianhydrides are employed to introduce molecularly quantized trap states into the conduction band of C3N4 to facilitate efficient charge separation, and to promote an enhanced photocatalytic CO2 reduction response. These modified C3N4 materials have been characterized structurally and spectroscopically for use as a support for Co-based SACs. In photocatalytic CO2 reduction studies, the Co SAC on naphthalene dianhydride-doped C3N4 exhibited the highest activity and selectivity toward CO production among the Co SACs tested in this work. The observed improvement in photocatalytic CO2-to-CO conversion activity correlates with trends in photoinduced charge separation, as revealed by photoluminescence spectroscopy.

AB - Graphitic carbon nitride (C3N4) has been widely explored as a photoactive support for single-atom catalysts (SACs). In this study, three different π-rich aromatic dianhydrides are employed to introduce molecularly quantized trap states into the conduction band of C3N4 to facilitate efficient charge separation, and to promote an enhanced photocatalytic CO2 reduction response. These modified C3N4 materials have been characterized structurally and spectroscopically for use as a support for Co-based SACs. In photocatalytic CO2 reduction studies, the Co SAC on naphthalene dianhydride-doped C3N4 exhibited the highest activity and selectivity toward CO production among the Co SACs tested in this work. The observed improvement in photocatalytic CO2-to-CO conversion activity correlates with trends in photoinduced charge separation, as revealed by photoluminescence spectroscopy.

KW - carbon nitride

KW - CO reduction

KW - cobalt

KW - photocatalysis

KW - single-atom catalyst

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U2 - 10.1021/acsaom.5c00019

DO - 10.1021/acsaom.5c00019

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JO - ACS Applied Optical Materials

JF - ACS Applied Optical Materials

IS - 4

ER -

Dianhydride-Modified Graphitic Carbon Nitride as a Support for Cobalt Single-Atom Photocatalysts

Abstract

ASJC Scopus Subject Areas

Keywords

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