Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain

Wittreich, Gerhard R.; Liu, Shizhong; Dauenhauer, Paul J.; Vlachos, Dionisios G.

doi:10.1126/sciadv.abl6576

Title: Catalytic resonance of ammonia synthesis by simulated dynamic ruthenium crystal strain

Journal Article · 26 January 2022 · Science Advances

DOI: https://doi.org/10.1126/sciadv.abl6576 · OSTI ID:1904786

^[1]; Liu, Shizhong ^[2];

^[3];

^[2]

Univ. of Delaware, Newark, DE (United States); Univ. of Delaware, Newark, DE (United States)
Univ. of Delaware, Newark, DE (United States)
Univ. of Minnesota, Minneapolis, MN (United States); Univ. of Delaware, Newark, DE (United States)

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 NH_x 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).

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Research Organization:: 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 Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Office (AMMTO)

Grant/Contract Number:: EE0007888; SC0001004

OSTI ID:: 1904786

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 4 Vol. 8; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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