Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain
Abstract
Ammonia affords dense storage for renewable energy as a fungible liquid fuel, provided it can be efficiently synthesized from hydrogen and nitrogen. In this work, the catalysis of ammonia synthesis was computationally explored beyond the Sabatier limit by dynamically straining a ruthenium crystal (±4%) at the resonant frequencies (102 to 105+ Hz) of N2 surface dissociation and hydrogenation. Density functional theory calculations at different strain conditions indicated that the energies of NHx surface intermediates and transition states scale linearly, allowing the description of ammonia synthesis at a continuum of strain conditions. A microkinetic model including multiple sites and surface diffusion between step and Ru(0001) terrace sites of varying ratios for nanoparticles of differing size revealed that dynamic strain yields catalytic ammonia synthesis conversion and turnover frequency comparable to industrial reactors (400°C, 200 atm) but at lower temperature (320°C) and an order of magnitude lower pressure (20 atm).
- Authors:
-
[1];
[2];
[1]
- Univ. of Delaware, Newark, DE (United States)
- Univ. of Minnesota, Minneapolis, MN (United States); Univ. of Delaware, Newark, DE (United States)
- Publication Date:
- Research Org.:
- American Institute of Chemical Engineers (AIChE), New York, NY (United States); Univ. of Delaware, Newark, DE (United States); Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO)
- OSTI Identifier:
- 1904786
- Grant/Contract Number:
- EE0007888; SC0001004
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 4; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 10 SYNTHETIC FUELS; Science & Technology - Other Topics
Citation Formats
Wittreich, Gerhard R., Liu, Shizhong, Dauenhauer, Paul J., and Vlachos, Dionisios G. Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain. United States: N. p., 2022.
Web. doi:10.1126/sciadv.abl6576.
Wittreich, Gerhard R., Liu, Shizhong, Dauenhauer, Paul J., & Vlachos, Dionisios G. Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain. United States. https://doi.org/10.1126/sciadv.abl6576
Wittreich, Gerhard R., Liu, Shizhong, Dauenhauer, Paul J., and Vlachos, Dionisios G. Wed .
"Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain". United States. https://doi.org/10.1126/sciadv.abl6576. https://www.osti.gov/servlets/purl/1904786.
@article{osti_1904786,
title = {Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain},
author = {Wittreich, Gerhard R. and Liu, Shizhong and Dauenhauer, Paul J. and Vlachos, Dionisios G.},
abstractNote = {Ammonia affords dense storage for renewable energy as a fungible liquid fuel, provided it can be efficiently synthesized from hydrogen and nitrogen. In this work, the catalysis of ammonia synthesis was computationally explored beyond the Sabatier limit by dynamically straining a ruthenium crystal (±4%) at the resonant frequencies (102 to 105+ Hz) of N2 surface dissociation and hydrogenation. Density functional theory calculations at different strain conditions indicated that the energies of NHx surface intermediates and transition states scale linearly, allowing the description of ammonia synthesis at a continuum of strain conditions. A microkinetic model including multiple sites and surface diffusion between step and Ru(0001) terrace sites of varying ratios for nanoparticles of differing size revealed that dynamic strain yields catalytic ammonia synthesis conversion and turnover frequency comparable to industrial reactors (400°C, 200 atm) but at lower temperature (320°C) and an order of magnitude lower pressure (20 atm).},
doi = {10.1126/sciadv.abl6576},
journal = {Science Advances},
number = 4,
volume = 8,
place = {United States},
year = {Wed Jan 26 00:00:00 EST 2022},
month = {Wed Jan 26 00:00:00 EST 2022}
}
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