Challenges in Electrocatalysis of Ammonia Oxidation on Platinum Surfaces: Discovering Reaction Pathways
dc.contributor.author | Venturini, Seiti I. | |
dc.contributor.author | Martins de Godoi, Denis R. [UNESP] | |
dc.contributor.author | Perez, Joelma | |
dc.contributor.institution | Universidade de São Paulo (USP) | |
dc.contributor.institution | Universidade Estadual Paulista (UNESP) | |
dc.date.accessioned | 2025-04-29T18:41:18Z | |
dc.date.issued | 2023-08-18 | |
dc.description.abstract | A deep understanding of the ammonia oxidation reaction (AOR) over platinum surfaces may facilitate the use of ammonia as a carbon-free source for energy storage and conversion. Herein, using an unprecedented experimental approach of combining online electrochemical mass spectrometry (OLEMS) and ion chromatography (IC) with high-area Pt/C surfaces, many AOR products were simultaneously detected and the variation in AOR selectivity depending on the surface conditions was demonstrated. In the low-potential region of 0.40-0.82 V, the adsorbed OH- was the dominant oxygenated surface species. The AOR onset potential was 0.40 V, and the surface intermediates were NHx,ads and N2Hy,ads, which were the main precursors of N2, considered a major product. N2H4, NO, and NH2OH were considered minor products in this potential region. In the high-potential region, from 0.82 V, adsorbed O2- was the main oxygenated surface species, owing to the strong interactions between OH- and oxidized Pt. We found that NO and N2O play a key role as reaction intermediates. Another remarkable result is the detection of HN3 as a gaseous product. NO2, N2H4, and NH2OH were considered the minor products. The nitrite and nitrate detected by IC were solution-phase products of the AOR at high potentials. The real-time identification of seven gaseous products, viz., N2, NO, N2H4, NH2OH, HN3, N2O, and NO2, and two solution-phase products, NO2- and NO3-, enabled us to propose AOR mechanistic pathways, opening more possibilities for the electrochemical generation of high-value-added nitrogenated products depending on Pt surface conditions. | en |
dc.description.affiliation | University of São Paulo (USP) São Carlos Institute of Chemistry, São Paulo | |
dc.description.affiliation | São Paulo State University (Unesp) Institute of Chemistry, São Paulo | |
dc.description.affiliationUnesp | São Paulo State University (Unesp) Institute of Chemistry, São Paulo | |
dc.format.extent | 10835-10845 | |
dc.identifier | http://dx.doi.org/10.1021/acscatal.3c00677 | |
dc.identifier.citation | ACS Catalysis, v. 13, n. 16, p. 10835-10845, 2023. | |
dc.identifier.doi | 10.1021/acscatal.3c00677 | |
dc.identifier.issn | 2155-5435 | |
dc.identifier.scopus | 2-s2.0-85168503655 | |
dc.identifier.uri | https://hdl.handle.net/11449/299049 | |
dc.language.iso | eng | |
dc.relation.ispartof | ACS Catalysis | |
dc.source | Scopus | |
dc.subject | ammonia oxidation reaction | |
dc.subject | electrocatalysis | |
dc.subject | OLEMS | |
dc.subject | platinum | |
dc.subject | reaction mechanism | |
dc.title | Challenges in Electrocatalysis of Ammonia Oxidation on Platinum Surfaces: Discovering Reaction Pathways | en |
dc.type | Artigo | pt |
dspace.entity.type | Publication | |
relation.isOrgUnitOfPublication | bc74a1ce-4c4c-4dad-8378-83962d76c4fd | |
relation.isOrgUnitOfPublication.latestForDiscovery | bc74a1ce-4c4c-4dad-8378-83962d76c4fd | |
unesp.author.orcid | 0000-0003-0604-3290[1] | |
unesp.author.orcid | 0000-0002-0462-1221[2] | |
unesp.author.orcid | 0000-0003-3307-4711[3] | |
unesp.campus | Universidade Estadual Paulista (UNESP), Instituto de Química, Araraquara | pt |