Nitrogenated Graphene Quantum Dot-Derived Copper Single-Atom Catalyst for Oxygen Reduction Reaction

Dawatage Shashika Madushani Perera; Prakhar Sharma; Ayanthi Thisera; Nadeesha Kothalawala; Matthew G. Boebinger; Beth S. Guiton; Doo Young Kim

doi:10.1021/acsomega.5c12972

Nitrogenated Graphene Quantum Dot-Derived Copper Single-Atom Catalyst for Oxygen Reduction Reaction

Dawatage Shashika Madushani Perera
, Prakhar Sharma
, Ayanthi Thisera
, Nadeesha Kothalawala
, Matthew G. Boebinger
, Beth S. Guiton
, Doo Young Kim

electron Microscopy and Microanalysis

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

Abstract

Despite the promise of fuel cells as sustainable energy conversion technologies, their widespread adoption is hindered by the high cost of platinum group metal (PGM) catalysts, particularly for catalyzing the oxygen reduction reaction (ORR) at the cathode. Here, we report copper-based single-atom catalysts (Cu-SACs) as cost-effective non-PGM alternatives for ORR. The catalysts were synthesized via simple pyrolysis of pyrene-derived amine-terminated graphene quantum dots (GQDs) in the presence of nitrogen and metal precursors. The abundant nitrogen functionality in GQDs effectively stabilized isolated Cu atoms during their conversion to porous carbon. A subsequent acid-washing step yielded a high density of atomically dispersed Cu active sites. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and high-resolution scanning transmission electron microscopy (HR-STEM) confirmed the effective incorporation of isolated Cu atoms into the carbon matrix through copper–nitrogen (Cu-N) coordination. Electrochemical measurements revealed excellent ORR activity with a dominant four-electron pathway. This synthetic strategy provides a practical route to developing economically viable, non-precious metal catalysts.

Original language	English
Pages (from-to)	12843-12851
Number of pages	9
Journal	ACS Omega
Volume	11
Issue number	7
DOIs	https://doi.org/10.1021/acsomega.5c12972
State	Published - Feb 24 2026

Funding

This work was supported by the National Science Foundation under grant OIA 2327349 (DYK, SP). Partial salary support was provided by the University of Kentucky Materials Science Research Priority Area (m-RPA) program (PS) and the College of Arts and Sciences (NLK), as well as by the U.S. Department of Energy under award number DE-SC0022315 (AT, BSG). Aberration-corrected HAADF STEM experimental work was conducted at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The authors gratefully acknowledge Professor Jason Unrine and his group in the Department of Plant and Soil Sciences at the University of Kentucky for assistance with ICP-MS measurements. XPS measurements were conducted at the Electron Microscopy Center (EMC), University of Kentucky.

Access to Document

10.1021/acsomega.5c12972

Cite this

@article{ab4e872976eb4b88a7f635c4273bfb72,

title = "Nitrogenated Graphene Quantum Dot-Derived Copper Single-Atom Catalyst for Oxygen Reduction Reaction",

abstract = "Despite the promise of fuel cells as sustainable energy conversion technologies, their widespread adoption is hindered by the high cost of platinum group metal (PGM) catalysts, particularly for catalyzing the oxygen reduction reaction (ORR) at the cathode. Here, we report copper-based single-atom catalysts (Cu-SACs) as cost-effective non-PGM alternatives for ORR. The catalysts were synthesized via simple pyrolysis of pyrene-derived amine-terminated graphene quantum dots (GQDs) in the presence of nitrogen and metal precursors. The abundant nitrogen functionality in GQDs effectively stabilized isolated Cu atoms during their conversion to porous carbon. A subsequent acid-washing step yielded a high density of atomically dispersed Cu active sites. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and high-resolution scanning transmission electron microscopy (HR-STEM) confirmed the effective incorporation of isolated Cu atoms into the carbon matrix through copper–nitrogen (Cu-N) coordination. Electrochemical measurements revealed excellent ORR activity with a dominant four-electron pathway. This synthetic strategy provides a practical route to developing economically viable, non-precious metal catalysts.",

author = "\{Shashika Madushani Perera\}, Dawatage and Prakhar Sharma and Ayanthi Thisera and Nadeesha Kothalawala and Boebinger, \{Matthew G.\} and Guiton, \{Beth S.\} and Kim, \{Doo Young\}",

note = "Publisher Copyright: {\textcopyright} 2026 The Authors. Published by American Chemical Society",

year = "2026",

month = feb,

day = "24",

doi = "10.1021/acsomega.5c12972",

language = "English",

volume = "11",

pages = "12843--12851",

journal = "ACS Omega",

issn = "2470-1343",

publisher = "American Chemical Society",

number = "7",

}

TY - JOUR

T1 - Nitrogenated Graphene Quantum Dot-Derived Copper Single-Atom Catalyst for Oxygen Reduction Reaction

AU - Shashika Madushani Perera, Dawatage

AU - Sharma, Prakhar

AU - Thisera, Ayanthi

AU - Kothalawala, Nadeesha

AU - Boebinger, Matthew G.

AU - Guiton, Beth S.

AU - Kim, Doo Young

PY - 2026/2/24

Y1 - 2026/2/24

N2 - Despite the promise of fuel cells as sustainable energy conversion technologies, their widespread adoption is hindered by the high cost of platinum group metal (PGM) catalysts, particularly for catalyzing the oxygen reduction reaction (ORR) at the cathode. Here, we report copper-based single-atom catalysts (Cu-SACs) as cost-effective non-PGM alternatives for ORR. The catalysts were synthesized via simple pyrolysis of pyrene-derived amine-terminated graphene quantum dots (GQDs) in the presence of nitrogen and metal precursors. The abundant nitrogen functionality in GQDs effectively stabilized isolated Cu atoms during their conversion to porous carbon. A subsequent acid-washing step yielded a high density of atomically dispersed Cu active sites. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and high-resolution scanning transmission electron microscopy (HR-STEM) confirmed the effective incorporation of isolated Cu atoms into the carbon matrix through copper–nitrogen (Cu-N) coordination. Electrochemical measurements revealed excellent ORR activity with a dominant four-electron pathway. This synthetic strategy provides a practical route to developing economically viable, non-precious metal catalysts.

AB - Despite the promise of fuel cells as sustainable energy conversion technologies, their widespread adoption is hindered by the high cost of platinum group metal (PGM) catalysts, particularly for catalyzing the oxygen reduction reaction (ORR) at the cathode. Here, we report copper-based single-atom catalysts (Cu-SACs) as cost-effective non-PGM alternatives for ORR. The catalysts were synthesized via simple pyrolysis of pyrene-derived amine-terminated graphene quantum dots (GQDs) in the presence of nitrogen and metal precursors. The abundant nitrogen functionality in GQDs effectively stabilized isolated Cu atoms during their conversion to porous carbon. A subsequent acid-washing step yielded a high density of atomically dispersed Cu active sites. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and high-resolution scanning transmission electron microscopy (HR-STEM) confirmed the effective incorporation of isolated Cu atoms into the carbon matrix through copper–nitrogen (Cu-N) coordination. Electrochemical measurements revealed excellent ORR activity with a dominant four-electron pathway. This synthetic strategy provides a practical route to developing economically viable, non-precious metal catalysts.

UR - https://www.scopus.com/pages/publications/105030982295

U2 - 10.1021/acsomega.5c12972

DO - 10.1021/acsomega.5c12972

M3 - Article

AN - SCOPUS:105030982295

SN - 2470-1343

VL - 11

SP - 12843

EP - 12851

JO - ACS Omega

JF - ACS Omega

IS - 7

ER -

Nitrogenated Graphene Quantum Dot-Derived Copper Single-Atom Catalyst for Oxygen Reduction Reaction

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this