A1 Journal article (refereed)
Coadsorption of NRR and HER Intermediates Determines the Performance of Ru-N4 toward Electrocatalytic N2 Reduction (2022)


Wu, T., Melander, M. M., & Honkala, K. (2022). Coadsorption of NRR and HER Intermediates Determines the Performance of Ru-N4 toward Electrocatalytic N2 Reduction. ACS Catalysis, 12(4), 2505-2512. https://doi.org/10.1021/acscatal.1c05820


JYU authors or editors


Publication details

All authors or editorsWu, Tongwei; Melander, Marko M.; Honkala, Karoliina

Journal or seriesACS Catalysis

ISSN2155-5435

eISSN2155-5435

Publication year2022

Publication date03/02/2022

Volume12

Issue number4

Pages range2505-2512

PublisherAmerican Chemical Society (ACS)

Publication countryUnited States

Publication languageEnglish

DOIhttps://doi.org/10.1021/acscatal.1c05820

Publication open accessOpenly available

Publication channel open accessPartially open access channel

Publication is parallel published (JYX)https://jyx.jyu.fi/handle/123456789/79690


Abstract

Electrochemical N2 reduction (NRR) to ammonia is seriously limited by the competing hydrogen evolution reaction (HER), but atomic-scale factors controlling HER/NRR competition are unknown. Herein we unveil the mechanism, thermodynamics, and kinetics determining the HER/NRR efficiency on the state-of-the-art NRR electrocatalyst, Ru-N4, using grand canonical ensemble density functional theory (GCE-DFT). We show that NRR/HER intermediates coadsorb on the catalyst where NRR intermediates suppress HER and selectivity is determined by the initial step forming *NNH or *H. Our results provide crucial insight into the complex NRR/HER competition, show the necessity of using GCE-DFT calculations, and suggest ways to improve NRR selectivity.


Keywordselectrolysisoxidation-reduction reactionhydrogenelectrochemistrycatalysiscatalysts

Free keywordshydrogen evolution reaction; electrochemical N2 reduction; grand canonical ensemble density functional theory


Contributing organizations


Related projects


Ministry reportingYes

Reporting Year2022

JUFO rating2


Last updated on 2024-14-06 at 23:46