Generalizable Trends in Electrochemical Protonation Barriers

التفاصيل البيبلوغرافية
العنوان: Generalizable Trends in Electrochemical Protonation Barriers
المؤلفون: Jens K. Nørskov, Georg Kastlunger, Karen Chan, Sudarshan Vijay, Anjli M. Patel
المصدر: The Journal of Physical Chemistry Letters. 12:5193-5200
بيانات النشر: American Chemical Society (ACS), 2021.
سنة النشر: 2021
مصطلحات موضوعية: Reaction mechanism, Materials science, Hydronium, Polyatomic ion, Protonation, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Bond order, 0104 chemical sciences, Catalysis, Monatomic ion, chemistry.chemical_compound, chemistry, Chemical physics, General Materials Science, Density functional theory, Physical and Theoretical Chemistry, 0210 nano-technology
الوصف: Predicting activation energies for reaction steps is essential for modeling catalytic processes, but accurate barrier simulations often require considerable computational expense, especially for electrochemical reactions. Given the challenges of barrier computations and the growing promise of electrochemical routes for various processes, generalizable energetic trends in electrochemistry can significantly aid in analyzing reaction networks and building microkinetic models. Herein, we employ density functional theory and machine learning nudged elastic band models to simulate electrochemical protonation of *C, *N, and *O monatomic adsorbates from hydronium on a series of transition metal surfaces. We observe a consistent trend of decreasing protonation reaction energies yet increasing activation barriers from *O to *N to *C. Analysis of bond orders and reaction pathways provides insight into the origin of the observed trends in protonation energetics. We hypothesize that these results are relevant for polyatomic adsorbates, which can simplify analysis of reaction mechanisms and inform catalyst design.
تدمد: 1948-7185
DOI: 10.1021/acs.jpclett.1c00800
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::c8ef5a32af5609b6faa7436d7792650b
https://doi.org/10.1021/acs.jpclett.1c00800
Rights: CLOSED
رقم الانضمام: edsair.doi.dedup.....c8ef5a32af5609b6faa7436d7792650b
قاعدة البيانات: OpenAIRE
الوصف
تدمد:19487185
DOI:10.1021/acs.jpclett.1c00800