A physical catalyst for the electrolysis of nitrogen to ammonia
Abstract
Ammonia synthesis consumes 3 to 5% of the world’s natural gas, making it a significant contributor to greenhouse gas emissions. Strategies for synthesizing ammonia that are not dependent on the energy-intensive and methane-based Haber-Bosch process are critically important for reducing global energy consumption and minimizing climate change. Motivated by a need to investigate novel nitrogen fixation mechanisms, we herein describe a highly textured physical catalyst, composed of N-doped carbon nanospikes, that electrochemically reduces dissolved N2 gas to ammonia in an aqueous electrolyte under ambient conditions. The Faradaic efficiency (FE) achieves 11.56 ± 0.85% at –1.19 V versus the reversible hydrogen electrode, and the maximum production rate is 97.18 ± 7.13 μg hour–1 cm–2. The catalyst contains no noble or rare metals but rather has a surface composed of sharp spikes, which concentrates the electric field at the tips, thereby promoting the electroreduction of dissolved N2 molecules near the electrode. The choice of electrolyte is also critically important because the reaction rate is dependent on the counterion type, suggesting a role in enhancing the electric field at the sharp spikes and increasing N2 concentration within the Stern layer. In conclusion, the energy efficiency of the reaction is estimated to be 5.25%more »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Georgia Inst. of Technology, Atlanta, GA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1468286
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 4; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Song, Yang, Johnson, Daniel A., Peng, Rui, Hensley, Dale K., Bonnesen, Peter V., Liang, Liangbo, Huang, Jingsong, Yang, Fengchang, Zhang, Fei, Qiao, Rui, Baddorf, Arthur P., Tschaplinski, Timothy J., Engle, Nancy L., Hatzell, Marta C., Wu, Zili, Cullen, David A., Meyer, III, Harry M., Sumpter, Bobby G., and Rondinone, Adam Justin. A physical catalyst for the electrolysis of nitrogen to ammonia. United States: N. p., 2018.
Web. doi:10.1126/sciadv.1700336.
Song, Yang, Johnson, Daniel A., Peng, Rui, Hensley, Dale K., Bonnesen, Peter V., Liang, Liangbo, Huang, Jingsong, Yang, Fengchang, Zhang, Fei, Qiao, Rui, Baddorf, Arthur P., Tschaplinski, Timothy J., Engle, Nancy L., Hatzell, Marta C., Wu, Zili, Cullen, David A., Meyer, III, Harry M., Sumpter, Bobby G., & Rondinone, Adam Justin. A physical catalyst for the electrolysis of nitrogen to ammonia. United States. https://doi.org/10.1126/sciadv.1700336
Song, Yang, Johnson, Daniel A., Peng, Rui, Hensley, Dale K., Bonnesen, Peter V., Liang, Liangbo, Huang, Jingsong, Yang, Fengchang, Zhang, Fei, Qiao, Rui, Baddorf, Arthur P., Tschaplinski, Timothy J., Engle, Nancy L., Hatzell, Marta C., Wu, Zili, Cullen, David A., Meyer, III, Harry M., Sumpter, Bobby G., and Rondinone, Adam Justin. Fri .
"A physical catalyst for the electrolysis of nitrogen to ammonia". United States. https://doi.org/10.1126/sciadv.1700336. https://www.osti.gov/servlets/purl/1468286.
@article{osti_1468286,
title = {A physical catalyst for the electrolysis of nitrogen to ammonia},
author = {Song, Yang and Johnson, Daniel A. and Peng, Rui and Hensley, Dale K. and Bonnesen, Peter V. and Liang, Liangbo and Huang, Jingsong and Yang, Fengchang and Zhang, Fei and Qiao, Rui and Baddorf, Arthur P. and Tschaplinski, Timothy J. and Engle, Nancy L. and Hatzell, Marta C. and Wu, Zili and Cullen, David A. and Meyer, III, Harry M. and Sumpter, Bobby G. and Rondinone, Adam Justin},
abstractNote = {Ammonia synthesis consumes 3 to 5% of the world’s natural gas, making it a significant contributor to greenhouse gas emissions. Strategies for synthesizing ammonia that are not dependent on the energy-intensive and methane-based Haber-Bosch process are critically important for reducing global energy consumption and minimizing climate change. Motivated by a need to investigate novel nitrogen fixation mechanisms, we herein describe a highly textured physical catalyst, composed of N-doped carbon nanospikes, that electrochemically reduces dissolved N2 gas to ammonia in an aqueous electrolyte under ambient conditions. The Faradaic efficiency (FE) achieves 11.56 ± 0.85% at –1.19 V versus the reversible hydrogen electrode, and the maximum production rate is 97.18 ± 7.13 μg hour–1 cm–2. The catalyst contains no noble or rare metals but rather has a surface composed of sharp spikes, which concentrates the electric field at the tips, thereby promoting the electroreduction of dissolved N2 molecules near the electrode. The choice of electrolyte is also critically important because the reaction rate is dependent on the counterion type, suggesting a role in enhancing the electric field at the sharp spikes and increasing N2 concentration within the Stern layer. In conclusion, the energy efficiency of the reaction is estimated to be 5.25% at the current FE of 11.56%.},
doi = {10.1126/sciadv.1700336},
journal = {Science Advances},
number = 4,
volume = 4,
place = {United States},
year = {Fri Apr 27 00:00:00 EDT 2018},
month = {Fri Apr 27 00:00:00 EDT 2018}
}
Web of Science
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Bi nanodendrites for efficient electrocatalytic N 2 fixation to NH 3 under ambient conditions
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Photocatalytic and electrocatalytic approaches towards atmospheric nitrogen reduction to ammonia under ambient conditions
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Electrochemical Synthesis of Ammonia: Recent Efforts and Future Outlook
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