Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering
Abstract
Ammonia, a key precursor for fertilizer production, convenient hydrogen carrier, and emerging clean fuel, plays a pivotal role in sustaining life on Earth. Currently, the main route for NH3 synthesis is by the heterogeneous catalytic Haber–Bosch process (N2+3 H2→2 NH3), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen–doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N2 into NH3 in an acidic aqueous solution under ambient conditions. The Faradaic efficiency and rate of production of NH3 on the NCM electrode reach 5.2 % and 0.08 g m–2 h–1, respectively. Functionalization of the NCM with Au nanoparticles dramatically enhances these performance metrics to 22 % and 0.36 gm–2 h–1, respectively. In conclusion, as this system offers the potential to be scaled to industrial levels it is highly likely that it might displace the century-old Haber–Bosch process.
- Authors:
-
[5];
[4]
- Nankai Univ., Tianjin (People's Republic of China)
- Univ. of Toronto, Toronto, ON (Canada); Soochow Univ., Jiangsu (People's Republic of China)
- The Chinese Academy of Sciences, Taiyuan (China)
- Univ. of Toronto, Toronto, ON (Canada)
- Temple Univ., Philadelphia, PA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Northwest Normal Univ., Lanzhou (People's Republic of China)
- Soochow Univ., Jiangsu (People's Republic of China)
- Stockholm Univ., Stockholm (Sweden)
- UNSW Australia, Sydney, NSW (Australia)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1476757
- Report Number(s):
- BNL-209144-2018-JAAM
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 38; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electrocatalysis; functionalization; nitrogen fixation; poly(ionic liquid); porous carbon membrane
Citation Formats
Wang, Hong, Wang, Lu, Wang, Qiang, Ye, Shuyang, Sun, Wei, Shao, Yue, Jiang, Zhiping, Qiao, Qiao, Zhu, Yimei, Song, Pengfei, Li, Debao, He, Le, Zhang, Xiaohong, Yuan, Jiayin, Wu, Tom, and Ozin, Geoffrey A. Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering. United States: N. p., 2018.
Web. doi:10.1002/anie.201805514.
Wang, Hong, Wang, Lu, Wang, Qiang, Ye, Shuyang, Sun, Wei, Shao, Yue, Jiang, Zhiping, Qiao, Qiao, Zhu, Yimei, Song, Pengfei, Li, Debao, He, Le, Zhang, Xiaohong, Yuan, Jiayin, Wu, Tom, & Ozin, Geoffrey A. Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering. United States. https://doi.org/10.1002/anie.201805514
Wang, Hong, Wang, Lu, Wang, Qiang, Ye, Shuyang, Sun, Wei, Shao, Yue, Jiang, Zhiping, Qiao, Qiao, Zhu, Yimei, Song, Pengfei, Li, Debao, He, Le, Zhang, Xiaohong, Yuan, Jiayin, Wu, Tom, and Ozin, Geoffrey A. Wed .
"Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering". United States. https://doi.org/10.1002/anie.201805514. https://www.osti.gov/servlets/purl/1476757.
@article{osti_1476757,
title = {Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering},
author = {Wang, Hong and Wang, Lu and Wang, Qiang and Ye, Shuyang and Sun, Wei and Shao, Yue and Jiang, Zhiping and Qiao, Qiao and Zhu, Yimei and Song, Pengfei and Li, Debao and He, Le and Zhang, Xiaohong and Yuan, Jiayin and Wu, Tom and Ozin, Geoffrey A.},
abstractNote = {Ammonia, a key precursor for fertilizer production, convenient hydrogen carrier, and emerging clean fuel, plays a pivotal role in sustaining life on Earth. Currently, the main route for NH3 synthesis is by the heterogeneous catalytic Haber–Bosch process (N2+3 H2→2 NH3), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen–doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N2 into NH3 in an acidic aqueous solution under ambient conditions. The Faradaic efficiency and rate of production of NH3 on the NCM electrode reach 5.2 % and 0.08 g m–2 h–1, respectively. Functionalization of the NCM with Au nanoparticles dramatically enhances these performance metrics to 22 % and 0.36 gm–2 h–1, respectively. In conclusion, as this system offers the potential to be scaled to industrial levels it is highly likely that it might displace the century-old Haber–Bosch process.},
doi = {10.1002/anie.201805514},
journal = {Angewandte Chemie (International Edition)},
number = 38,
volume = 57,
place = {United States},
year = {Wed Jun 20 00:00:00 EDT 2018},
month = {Wed Jun 20 00:00:00 EDT 2018}
}
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Figures / Tables:
Figure 1: a)-c), Scheme illustrating the synthetic route to the NCM. Image (a) depicts a homogeneous dispersion of CNTs in a solution of PCMVImTf2N and PAA in DMF; Image (b) is a PCMVImTf2N/PAA/CNT hybrid membrane; Image (c) is a NCM prepared from pyrolysis of sample in (b); d), SEM imagemore »
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