Bottom up synthesis of boron-doped graphene for stable intermediate temperature fuel cell electrodes
Abstract
The high surface area and electrical conductivity of few-layered graphene would make it an ideal catalyst support and electrode in fuel cells apart from its susceptibility to oxidative corrosion. Here we report the single-step, bottom-up synthesis of oxidation-resistant boron-doped graphene and show its increased stability in the aggressive electrochemical environment of intermediate temperature solid acid fuel cells (SAFCs). Boron was shown to alter the growth mode of single walled carbon nanohorns by laser vaporization to produce high yields of thin (<20 layer) boron-doped (2–3 at.%) crystalline flakes of turbostratic graphene (B-GLF). Alternatively, adding partial pressures of hydrogen less effectively shifted the growth mode of SWCNHs toward planar, turbostratic graphene-like flakes (GLFs). Thermogravimetric analysis indicates that boron-doping enhances the oxidation resistance of few-layer GLFs by >140 °C, with large fractions of multilayered B-GLFs surviving 10 °C/min ramps to 1000 °C. These B-GLFs provided a stable Pt catalyst support and electrode over 40 h operation in SAFCs with cesium dihydrogen phosphate electrolyte operating at 250 °C, as opposed to undoped GLFs or SWCNHs which were nearly completely consumed. Furthermore, the facile synthesis and oxidation-resistant properties of boron-doped GLF appear promising for graphene applications in oxidizing environments.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1];
[1]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1489107
- Alternate Identifier(s):
- OSTI ID: 1547093
- Grant/Contract Number:
- AC05-00OR22725; AR0000499
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Carbon
- Additional Journal Information:
- Journal Volume: 123; Journal Issue: C; Journal ID: ISSN 0008-6223
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; CsH2PO4; Single wall carbon nanohorns; Solid acid fuel cells; Few-layer graphene; Boron doped carbon; Boron; Pulsed laser vaporization
Citation Formats
Tennyson, Wesley D., Tian, Mengkun, Papandrew, Alexander B., Rouleau, Christopher M., Puretzky, Alexander A., Sneed, Brian T., More, Karren Leslie, Veith, Gabriel M., Duscher, Gerd J. M., Zawodzinski, Thomas A., and Geohegan, David B. Bottom up synthesis of boron-doped graphene for stable intermediate temperature fuel cell electrodes. United States: N. p., 2017.
Web. doi:10.1016/j.carbon.2017.08.002.
Tennyson, Wesley D., Tian, Mengkun, Papandrew, Alexander B., Rouleau, Christopher M., Puretzky, Alexander A., Sneed, Brian T., More, Karren Leslie, Veith, Gabriel M., Duscher, Gerd J. M., Zawodzinski, Thomas A., & Geohegan, David B. Bottom up synthesis of boron-doped graphene for stable intermediate temperature fuel cell electrodes. United States. https://doi.org/10.1016/j.carbon.2017.08.002
Tennyson, Wesley D., Tian, Mengkun, Papandrew, Alexander B., Rouleau, Christopher M., Puretzky, Alexander A., Sneed, Brian T., More, Karren Leslie, Veith, Gabriel M., Duscher, Gerd J. M., Zawodzinski, Thomas A., and Geohegan, David B. Fri .
"Bottom up synthesis of boron-doped graphene for stable intermediate temperature fuel cell electrodes". United States. https://doi.org/10.1016/j.carbon.2017.08.002. https://www.osti.gov/servlets/purl/1489107.
@article{osti_1489107,
title = {Bottom up synthesis of boron-doped graphene for stable intermediate temperature fuel cell electrodes},
author = {Tennyson, Wesley D. and Tian, Mengkun and Papandrew, Alexander B. and Rouleau, Christopher M. and Puretzky, Alexander A. and Sneed, Brian T. and More, Karren Leslie and Veith, Gabriel M. and Duscher, Gerd J. M. and Zawodzinski, Thomas A. and Geohegan, David B.},
abstractNote = {The high surface area and electrical conductivity of few-layered graphene would make it an ideal catalyst support and electrode in fuel cells apart from its susceptibility to oxidative corrosion. Here we report the single-step, bottom-up synthesis of oxidation-resistant boron-doped graphene and show its increased stability in the aggressive electrochemical environment of intermediate temperature solid acid fuel cells (SAFCs). Boron was shown to alter the growth mode of single walled carbon nanohorns by laser vaporization to produce high yields of thin (<20 layer) boron-doped (2–3 at.%) crystalline flakes of turbostratic graphene (B-GLF). Alternatively, adding partial pressures of hydrogen less effectively shifted the growth mode of SWCNHs toward planar, turbostratic graphene-like flakes (GLFs). Thermogravimetric analysis indicates that boron-doping enhances the oxidation resistance of few-layer GLFs by >140 °C, with large fractions of multilayered B-GLFs surviving 10 °C/min ramps to 1000 °C. These B-GLFs provided a stable Pt catalyst support and electrode over 40 h operation in SAFCs with cesium dihydrogen phosphate electrolyte operating at 250 °C, as opposed to undoped GLFs or SWCNHs which were nearly completely consumed. Furthermore, the facile synthesis and oxidation-resistant properties of boron-doped GLF appear promising for graphene applications in oxidizing environments.},
doi = {10.1016/j.carbon.2017.08.002},
journal = {Carbon},
number = C,
volume = 123,
place = {United States},
year = {Fri Aug 04 00:00:00 EDT 2017},
month = {Fri Aug 04 00:00:00 EDT 2017}
}
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Figure 1.: Single-wall carbon nanohorns aggregates produced by pulsed laser vaporization (PLV) (a) SEM image of the SWCNH aggregates produced by 20 msec PLV of carbon in Ar at 1100°C, 760 Torr, and 5 Hz repetition rate. (b) TEM of the SWCNH aggregates. (c) HRTEM of protruding SWCNH from anmore »
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Works referencing / citing this record:
In situ determination of the electrochemically active platinum surface area: key to improvement of solid acid fuel cells
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