Subsurface Nitrogen Dissociation Kinetics in Lithium Metal from Metadynamics

Ludwig, Thomas; Singh, Aayush R.; Nørskov, Jens K.

doi:10.1021/acs.jpcc.0c09108

Title: Subsurface Nitrogen Dissociation Kinetics in Lithium Metal from Metadynamics

Journal Article · Thu Nov 19 00:00:00 EST 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c09108· OSTI ID:1768395

^[1];

^[2]

SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
Technical Univ. of Denmark, Kongens Lyngby (Denmark)

The dissociation of molecular nitrogen in lithium is of interest for several promising technologies, such as the catalytic synthesis of ammonia in ambient or mild conditions. In this work we simulate nitrogen dissociation in the lithium BCC (110) surface at ambient and elevated temperatures using density functional theory (DFT) metadynamics simulations. The rate constants at temperatures of 300, 400, and 500 K are calculated by statistical analysis of the reaction time distributions from the accelerated simulations. This approach finds and estimates rate constants for transition pathways out of the initial state; the required input is the stable initial state and a reasonable choice of collective variable. A single collective variable is used in this case: the N–N distance. The results are robust to changes in metadynamics parameters, and the reaction time distributions follow the expected exponential distribution. We show that the metadynamics-derived rate constants are in agreement with results from the conventional harmonic approximation approach using a climbing image nudged elastic band (NEB) transition state search. The reaction barriers from metadynamics and the NEB/harmonic approximation agree to within 0.02–0.04 eV at all temperatures studied. This paper demonstrates that the harmonic approximation provides an accurate description of the rate constants for nitrogen dissociation in lithium metal, even at temperatures near or above the melting point of lithium, lending credence to previous and future theoretical studies using this approximation. Moreover, this work demonstrates a step toward the automated exploration and discovery of reaction mechanisms and associated rate constants for elementary surface-catalyzed reactions using DFT-based metadynamics.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-76SF00515; 9455; FG02-97ER25308

OSTI ID:: 1768395

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 48; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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