Pyridinic nitrogen induced compressed bilayer graphene for oxygen reduction reaction

Navid Solati; Mehmet Çankaya; Abdullah Kahraman; Kaan Şimşek; Charles James Titus; Sang Jun Lee; Dennis Nordlund; Hirohito Ogasawara; Adem Tekin; Sarp Kaya

doi:10.1016/j.mtener.2023.101323

Pyridinic nitrogen induced compressed bilayer graphene for oxygen reduction reaction

Navid Solati
, Mehmet Çankaya
, Abdullah Kahraman
, Kaan Şimşek
, Charles James Titus
, Sang Jun Lee
, Dennis Nordlund
, Hirohito Ogasawara
, Adem Tekin^*
, Sarp Kaya^*

^*Corresponding author for this work

Informatics Institute

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

11 Citations (Scopus)

Abstract

Despite the emergence of nitrogen-doped graphene as a noble-metal free electrocatalyst for oxygen reduction reaction, its participation in the electrochemical conversion mechanism is not well-established. In the present study, functionalities of the nitrogen species on the oxygen reduction activity of bilayer graphene were investigated by combining atom-specific X-ray spectroscopy, Raman spectroscopy, and density functional theory calculations with electrochemical activity tests in alkaline media. Among various nitrogen species, pyridinic nitrogen as the dominant species improved the electrochemical activity of bilayer graphene, which was followed by graphene bilayers doped with graphitic nitrogen in majority. Polarization curves revealed a significantly high electrocatalytic oxygen reduction activity of the nitrogen-doped bilayer graphene where the pyridinic nitrogen was the major dopant. This improved activity was confirmed by the lowest overpotential and Tafel slope (78.9 mV/dec). The enhanced interaction of graphene bilayers doped with pyridinic nitrogen is shown to be the main reason for this improvement.

Original language	English
Article number	101323
Journal	Materials Today Energy
Volume	35
DOIs	https://doi.org/10.1016/j.mtener.2023.101323
Publication status	Published - Jul 2023

Bibliographical note

Publisher Copyright:
© 2023 Elsevier Ltd

Funding

The use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The N.S. M.Ç. A.T. and S.K. would like to thank The Scientific and Technical Research Council of Türkiye (TUBITAK) for support (Grant number: 217M540 and 113Z654). The authors thank KUYTAM for the characterization measurements and the Quantum Sensors Project group at NIST Boulder, CO for their development and support of the TES spectrometer at SSRL BL 10-1. The use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The N.S., M.Ç., A.T., and S.K. would like to thank The Scientific and Technical Research Council of Türkiye (TUBITAK) for support (Grant number: 217M540 and 113Z654 ). The authors thank KUYTAM for the characterization measurements and the Quantum Sensors Project group at NIST Boulder, CO for their development and support of the TES spectrometer at SSRL BL 10-1.

Funders	Funder number
KUYTAM
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC02-76SF00515
Türkiye Bilimsel ve Teknolojik Araştırma Kurumu	217M540, 113Z654

Keywords

DFT
Functionalized graphene
Nitrogen doping
ORR
X-ray spectroscopy

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10.1016/j.mtener.2023.101323

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title = "Pyridinic nitrogen induced compressed bilayer graphene for oxygen reduction reaction",

abstract = "Despite the emergence of nitrogen-doped graphene as a noble-metal free electrocatalyst for oxygen reduction reaction, its participation in the electrochemical conversion mechanism is not well-established. In the present study, functionalities of the nitrogen species on the oxygen reduction activity of bilayer graphene were investigated by combining atom-specific X-ray spectroscopy, Raman spectroscopy, and density functional theory calculations with electrochemical activity tests in alkaline media. Among various nitrogen species, pyridinic nitrogen as the dominant species improved the electrochemical activity of bilayer graphene, which was followed by graphene bilayers doped with graphitic nitrogen in majority. Polarization curves revealed a significantly high electrocatalytic oxygen reduction activity of the nitrogen-doped bilayer graphene where the pyridinic nitrogen was the major dopant. This improved activity was confirmed by the lowest overpotential and Tafel slope (78.9 mV/dec). The enhanced interaction of graphene bilayers doped with pyridinic nitrogen is shown to be the main reason for this improvement.",

keywords = "DFT, Functionalized graphene, Nitrogen doping, ORR, X-ray spectroscopy",

author = "Navid Solati and Mehmet {\c C}ankaya and Abdullah Kahraman and Kaan {\c S}im{\c s}ek and Titus, \{Charles James\} and Lee, \{Sang Jun\} and Dennis Nordlund and Hirohito Ogasawara and Adem Tekin and Sarp Kaya",

note = "Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

year = "2023",

month = jul,

doi = "10.1016/j.mtener.2023.101323",

language = "English",

volume = "35",

journal = "Materials Today Energy",

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T1 - Pyridinic nitrogen induced compressed bilayer graphene for oxygen reduction reaction

AU - Solati, Navid

AU - Çankaya, Mehmet

AU - Kahraman, Abdullah

AU - Şimşek, Kaan

AU - Titus, Charles James

AU - Lee, Sang Jun

AU - Nordlund, Dennis

AU - Ogasawara, Hirohito

AU - Tekin, Adem

AU - Kaya, Sarp

PY - 2023/7

Y1 - 2023/7

N2 - Despite the emergence of nitrogen-doped graphene as a noble-metal free electrocatalyst for oxygen reduction reaction, its participation in the electrochemical conversion mechanism is not well-established. In the present study, functionalities of the nitrogen species on the oxygen reduction activity of bilayer graphene were investigated by combining atom-specific X-ray spectroscopy, Raman spectroscopy, and density functional theory calculations with electrochemical activity tests in alkaline media. Among various nitrogen species, pyridinic nitrogen as the dominant species improved the electrochemical activity of bilayer graphene, which was followed by graphene bilayers doped with graphitic nitrogen in majority. Polarization curves revealed a significantly high electrocatalytic oxygen reduction activity of the nitrogen-doped bilayer graphene where the pyridinic nitrogen was the major dopant. This improved activity was confirmed by the lowest overpotential and Tafel slope (78.9 mV/dec). The enhanced interaction of graphene bilayers doped with pyridinic nitrogen is shown to be the main reason for this improvement.

AB - Despite the emergence of nitrogen-doped graphene as a noble-metal free electrocatalyst for oxygen reduction reaction, its participation in the electrochemical conversion mechanism is not well-established. In the present study, functionalities of the nitrogen species on the oxygen reduction activity of bilayer graphene were investigated by combining atom-specific X-ray spectroscopy, Raman spectroscopy, and density functional theory calculations with electrochemical activity tests in alkaline media. Among various nitrogen species, pyridinic nitrogen as the dominant species improved the electrochemical activity of bilayer graphene, which was followed by graphene bilayers doped with graphitic nitrogen in majority. Polarization curves revealed a significantly high electrocatalytic oxygen reduction activity of the nitrogen-doped bilayer graphene where the pyridinic nitrogen was the major dopant. This improved activity was confirmed by the lowest overpotential and Tafel slope (78.9 mV/dec). The enhanced interaction of graphene bilayers doped with pyridinic nitrogen is shown to be the main reason for this improvement.

KW - DFT

KW - Functionalized graphene

KW - Nitrogen doping

KW - ORR

KW - X-ray spectroscopy

UR - https://www.scopus.com/pages/publications/85159858375

U2 - 10.1016/j.mtener.2023.101323

DO - 10.1016/j.mtener.2023.101323

M3 - Article

AN - SCOPUS:85159858375

SN - 2468-6069

VL - 35

JO - Materials Today Energy

JF - Materials Today Energy

M1 - 101323

ER -

Pyridinic nitrogen induced compressed bilayer graphene for oxygen reduction reaction

Abstract

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Keywords

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