Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis
Abstract
Controlling active sites of metal-free catalysts is an important strategy to enhance activity of the oxygen evolution reaction (OER). We made many attempts have been made to develop metal-free catalysts, but the lack of understanding of active-sites at the atomic-level has slowed the design of highly active and stable metal-free catalysts. We also developed a sequential two-step strategy to dope sulfur into carbon nanotube–graphene nanolobes. This bidoping strategy introduces stable sulfur–carbon active-sites. Fluorescence emission of the sulfur K-edge by X-ray absorption near edge spectroscopy (XANES) and scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) mapping and spectra confirm that increasing the incorporation of heterocyclic sulfur into the carbon ring of CNTs not only enhances OER activity with an overpotential of 350 mV at a current density of 10 mA cm-2, but also retains 100% of stability after 75 h. Furthermore, the bidoped sulfur carbon nanotube–graphene nanolobes behave like the state-of-the-art catalysts for OER but outperform those systems in terms of turnover frequency (TOF) which is two orders of magnitude greater than (20% Ir/C) at 400 mV overpotential with very high mass activity 1000 mA cm-2 at 570 mV. Moreover, the sulfur bidoping strategy shows high catalytic activity for themore »
- Authors:
-
- Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry and Inst. of Materials Science; Tanta Univ. (Egypt). Dept. of Chemistry
- Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry; Tanta Univ. (Egypt). Dept. of Chemistry
- Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton NY 11973 USA; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry
- Photon Science Directorate, Brookhaven National Laboratory, Upton NY 11973 USA; Brookhaven National Lab. (BNL), Upton, NY (United States)
- Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry and Inst. of Materials Science
- Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry and Inst. of Materials Science and Chemical and Biomolecular Engineering
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1336156
- Report Number(s):
- BNL-112670-2016-JA
Journal ID: ISSN 1614-6832; KC0403020
- Grant/Contract Number:
- SC00112704; FG02-86ER13622.A000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 5; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Sulfur-Doped Carbon; oxygen reduction; Center for Functional Nanomaterials
Citation Formats
El-Sawy, Abdelhamid M., Mosa, Islam M., Su, Dong, Guild, Curtis J., Khalid, Syed, Joesten, Raymond, Rusling, James F., and Suib, Steven L. Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis. United States: N. p., 2015.
Web. doi:10.1002/aenm.201501966.
El-Sawy, Abdelhamid M., Mosa, Islam M., Su, Dong, Guild, Curtis J., Khalid, Syed, Joesten, Raymond, Rusling, James F., & Suib, Steven L. Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis. United States. https://doi.org/10.1002/aenm.201501966
El-Sawy, Abdelhamid M., Mosa, Islam M., Su, Dong, Guild, Curtis J., Khalid, Syed, Joesten, Raymond, Rusling, James F., and Suib, Steven L. Thu .
"Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis". United States. https://doi.org/10.1002/aenm.201501966. https://www.osti.gov/servlets/purl/1336156.
@article{osti_1336156,
title = {Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis},
author = {El-Sawy, Abdelhamid M. and Mosa, Islam M. and Su, Dong and Guild, Curtis J. and Khalid, Syed and Joesten, Raymond and Rusling, James F. and Suib, Steven L.},
abstractNote = {Controlling active sites of metal-free catalysts is an important strategy to enhance activity of the oxygen evolution reaction (OER). We made many attempts have been made to develop metal-free catalysts, but the lack of understanding of active-sites at the atomic-level has slowed the design of highly active and stable metal-free catalysts. We also developed a sequential two-step strategy to dope sulfur into carbon nanotube–graphene nanolobes. This bidoping strategy introduces stable sulfur–carbon active-sites. Fluorescence emission of the sulfur K-edge by X-ray absorption near edge spectroscopy (XANES) and scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) mapping and spectra confirm that increasing the incorporation of heterocyclic sulfur into the carbon ring of CNTs not only enhances OER activity with an overpotential of 350 mV at a current density of 10 mA cm-2, but also retains 100% of stability after 75 h. Furthermore, the bidoped sulfur carbon nanotube–graphene nanolobes behave like the state-of-the-art catalysts for OER but outperform those systems in terms of turnover frequency (TOF) which is two orders of magnitude greater than (20% Ir/C) at 400 mV overpotential with very high mass activity 1000 mA cm-2 at 570 mV. Moreover, the sulfur bidoping strategy shows high catalytic activity for the oxygen reduction reaction (ORR). Stable bifunctional (ORR and OER) catalysts are low cost, and light-weight bidoped sulfur carbon nanotubes are potential candidates for next-generation metal-free regenerative fuel cells.},
doi = {10.1002/aenm.201501966},
journal = {Advanced Energy Materials},
number = 5,
volume = 6,
place = {United States},
year = {Thu Dec 03 00:00:00 EST 2015},
month = {Thu Dec 03 00:00:00 EST 2015}
}
Web of Science
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Bifunctional Oxygen Electrocatalysts for Lithium−Oxygen Batteries
journal, February 2019
- Bae, Youngjoon; Park, Hyeokjun; Ko, Youngmin
- Batteries & Supercaps, Vol. 2, Issue 4