Advanced search
Start date
(Reference retrieved automatically from Web of Science through information on FAPESP grant and its corresponding number as mentioned in the publication by the authors.)

X-ray Photoelectron Fingerprints of High-Valence Ruthenium-Oxo Complexes along the Oxidation Reaction Pathway in an Aqueous Environment

Full text
Show less -
Silva, Jose Luis [1] ; Unger, Isaak [2] ; Matias, Tiago Araujo [3] ; Franco, Leandro Rezende [4] ; Damas, Giane [1] ; Costa, Luciano T. [5] ; Toledo, Kalil C. F. [3] ; Rocha, Tulio C. R. [6] ; de Brito, Arnaldo Naves [7] ; Saak, Clara-Magdalena [2] ; Coutinho, Kaline [4] ; Araki, Koiti [3] ; Bjorneholm, Olle [2] ; Brena, Barbara [1] ; Araujo, C. Moyses [1]
Total Authors: 15
[1] Uppsala Univ, Dept Phys & Astron, Mat Theory Div, Box S16, S-75120 Uppsala - Sweden
[2] Uppsala Univ, Dept Phys & Astron, Mol & Condensed Matter Phys Div, Box 516, S-75120 Uppsala - Sweden
[3] Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, Av Lineu Prestes 748, BR-05508000 Butanta, SP - Brazil
[4] Univ Sao Paulo, Inst Fis, BR-05508090 Sao Paulo, SP - Brazil
[5] Univ Fed Fluminense, Dept Fisicoquim, Inst Quim, Outeiro Sao Joao Batista S-N, BR-24020150 Niteroi, RJ - Brazil
[6] Brazilian Ctr Res Energy & Mat CNPEM, Brazilian Synchrotron Light Lab LNLS, POB 6192, BR-13083970 Campinas, SP - Brazil
[7] Univ Estadual Campinas, Inst Phys Gleb Wataghin, BR-13083859 Campinas, SP - Brazil
Total Affiliations: 7
Document type: Journal article
Source: Journal of Physical Chemistry Letters; v. 10, n. 24, p. 7636-7643, DEC 19 2019.
Web of Science Citations: 0

Recent advances in operando-synchrotron-based X-ray techniques are making it possible to address fundamental questions related to complex proton-coupled electron transfer reactions, for instance, the electrocatalytic water splitting process. However, it is still a grand challenge to assess the ability of the different techniques to characterize the relevant intermediates, with minimal interference on the reaction mechanism. To this end, we have developed a novel methodology employing X-ray photoelectron spectroscopy (XPS) in connection with the liquid-jet approach to probe the electrochemical properties of a model electrocatalyst, {[}Ru-II(bpy)(2)(py)-(OH2)](2+), in an aqueous environment. There is a unique fingerprint of the extremely important higher-valence ruthenium-oxo species in the XPS spectra along the oxidation reaction pathway. Furthermore, a sequential method combining quantum mechanics and molecular mechanics is used to illuminate the underlying physical chemistry of such systems. This study provides the basis for the future development of in-operando XPS techniques for water oxidation reactions. (AU)

FAPESP's process: 18/04523-1 - Activation of OER catalysts based on binuclear ruthenium complexes by hydrogen bonding groups
Grantee:Kalil Cristhian Figueiredo Toledo
Support type: Scholarships in Brazil - Post-Doctorate
FAPESP's process: 17/11986-5 - Research Division 1 - dense energy carriers
Grantee:Ana Flávia Nogueira
Support type: Research Grants - Research Centers in Engineering Program
FAPESP's process: 13/24725-4 - Supramolecular chemistry and nanotechnology
Grantee:Henrique Eisi Toma
Support type: Research Projects - Thematic Grants
FAPESP's process: 17/11631-2 - Computational material science and chemistry
Grantee:Juarez Lopes Ferreira da Silva
Support type: Research Grants - Research Centers in Engineering Program
FAPESP's process: 17/50129-0 - Hybrid nanomaterials and nanosystems for solar fuel production
Grantee:Koiti Araki
Support type: Regular Research Grants