Sulfur-Modified Graphitic Carbon Nitride Nanostructures as an Efficient Electrocatalyst for Water Oxidation

Vinayak S. Kale; Uk Sim; Jiwoong Yang; Kyoungsuk Jin; Sue In Chae; Woo Je Chang; Arun Kumar Sinha; Heonjin Ha; Chan Cuk Hwang; Junghyun An; Hyo Ki Hong; Zonghoon Lee; Ki Tae Nam; Taeghwan Hyeon

doi:10.1002/smll.201603893

Sulfur-Modified Graphitic Carbon Nitride Nanostructures as an Efficient Electrocatalyst for Water Oxidation

Vinayak S. Kale
, Uk Sim
, Jiwoong Yang
, Kyoungsuk Jin
, Sue In Chae
, Woo Je Chang
, Arun Kumar Sinha
, Heonjin Ha
, Chan Cuk Hwang
, Junghyun An
, Hyo Ki Hong
, Zonghoon Lee
, Ki Tae Nam^*
, Taeghwan Hyeon

^*Corresponding author for this work

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

60 Citations (Scopus)

Abstract

There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN _x) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN _x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN _x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm⁻² and a Tafel slope of 120 mV dec⁻¹ with long-term durability of 91.2% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.

Original language	English
Article number	1603893
Journal	Small
Volume	13
Issue number	17
DOIs	https://doi.org/10.1002/smll.201603893
Publication status	Published - 2017 May 3
Externally published	Yes

Bibliographical note

Funding Information:
V.S.K. and U.S. contributed equally to this work. The authors acknowledge financial support from the Institute for Basic Science in the Republic of Korea (IBS-R006-D1) (T.H.), the Global Frontier R&D Program on Center for Multiscale Energy System (2011-0031571) funded by the Ministry of Science, ICT & Future, Korea through the Research Institute of Advanced Materials (RIAM) and by KIST Institutional Program (0543-20160004) (K.T.N.), the financial support by the NRF through the SRC Center for Topological Matter (No. 2011-0030787), the experiments at PLS were supported in part by MSIP and POSTECH (C.-C.H.), and the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIP) (No. 2015R1A2A2A01006992) (Z.L.).

Publisher Copyright:
© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

electrocatalysis
graphitic carbon nitride
nanostructures
oxygen evolution reaction

ASJC Scopus subject areas

General Chemistry
General Materials Science
Biotechnology
Biomaterials

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10.1002/smll.201603893

Cite this

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title = "Sulfur-Modified Graphitic Carbon Nitride Nanostructures as an Efficient Electrocatalyst for Water Oxidation",

abstract = "There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN x) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm−2 and a Tafel slope of 120 mV dec−1 with long-term durability of 91.2\% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.",

keywords = "electrocatalysis, graphitic carbon nitride, nanostructures, oxygen evolution reaction",

author = "Kale, \{Vinayak S.\} and Uk Sim and Jiwoong Yang and Kyoungsuk Jin and Chae, \{Sue In\} and Chang, \{Woo Je\} and Sinha, \{Arun Kumar\} and Heonjin Ha and Hwang, \{Chan Cuk\} and Junghyun An and Hong, \{Hyo Ki\} and Zonghoon Lee and Nam, \{Ki Tae\} and Taeghwan Hyeon",

note = "Funding Information: V.S.K. and U.S. contributed equally to this work. The authors acknowledge financial support from the Institute for Basic Science in the Republic of Korea (IBS-R006-D1) (T.H.), the Global Frontier R\&D Program on Center for Multiscale Energy System (2011-0031571) funded by the Ministry of Science, ICT \& Future, Korea through the Research Institute of Advanced Materials (RIAM) and by KIST Institutional Program (0543-20160004) (K.T.N.), the financial support by the NRF through the SRC Center for Topological Matter (No. 2011-0030787), the experiments at PLS were supported in part by MSIP and POSTECH (C.-C.H.), and the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIP) (No. 2015R1A2A2A01006992) (Z.L.). Publisher Copyright: {\textcopyright} 2017 WILEY-VCH Verlag GmbH \& Co. KGaA, Weinheim",

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month = may,

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doi = "10.1002/smll.201603893",

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AU - Kale, Vinayak S.

AU - Sim, Uk

AU - Yang, Jiwoong

AU - Jin, Kyoungsuk

AU - Chae, Sue In

AU - Chang, Woo Je

AU - Sinha, Arun Kumar

AU - Ha, Heonjin

AU - Hwang, Chan Cuk

AU - An, Junghyun

AU - Hong, Hyo Ki

AU - Lee, Zonghoon

AU - Nam, Ki Tae

AU - Hyeon, Taeghwan

N1 - Funding Information: V.S.K. and U.S. contributed equally to this work. The authors acknowledge financial support from the Institute for Basic Science in the Republic of Korea (IBS-R006-D1) (T.H.), the Global Frontier R&D Program on Center for Multiscale Energy System (2011-0031571) funded by the Ministry of Science, ICT & Future, Korea through the Research Institute of Advanced Materials (RIAM) and by KIST Institutional Program (0543-20160004) (K.T.N.), the financial support by the NRF through the SRC Center for Topological Matter (No. 2011-0030787), the experiments at PLS were supported in part by MSIP and POSTECH (C.-C.H.), and the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIP) (No. 2015R1A2A2A01006992) (Z.L.). Publisher Copyright: © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2017/5/3

Y1 - 2017/5/3

N2 - There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN x) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm−2 and a Tafel slope of 120 mV dec−1 with long-term durability of 91.2% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.

AB - There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN x) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm−2 and a Tafel slope of 120 mV dec−1 with long-term durability of 91.2% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.

KW - electrocatalysis

KW - graphitic carbon nitride

KW - nanostructures

KW - oxygen evolution reaction

UR - https://www.scopus.com/pages/publications/85013449870

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DO - 10.1002/smll.201603893

M3 - Article

C2 - 28218825

AN - SCOPUS:85013449870

SN - 1613-6810

VL - 13

JO - Small

JF - Small

IS - 17

M1 - 1603893

ER -

Sulfur-Modified Graphitic Carbon Nitride Nanostructures as an Efficient Electrocatalyst for Water Oxidation

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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