A highly efficient Ir-catalyst for the solventless dehydrogenation of formic acid: the key role of an N-heterocyclic olefin

Iturmendi, Amaia ; Iglesias, Manuel (Universidad de Zaragoza) ; Munarriz, Julen (Universidad de Zaragoza) ; Polo, Víctor (Universidad de Zaragoza) ; Passarelli, Vicenzo ; Perez-Torrente, Jesús J. (Universidad de Zaragoza) ; Oro, Luis A. (Universidad de Zaragoza)

Resumen: The use of formic acid as a hydrogen energy carrier has sparked the interest of the scientific community in the development of catalysts that promote its selective dehydrogenation. Most of the catalysts so far reported require the use of solvents that reduce the hydrogen density of the mixture and may even damage the fuel cell electrode materials. We present here a sturdy iridium catalyst that features a PCP ligand based on an N-heterocyclic olefin (NHO) scaffold, which is remarkably active for the dehydrogenation of neat formic acid. Related complexes that present bis-phosphine ligands without an NHO donor moiety give rise to noticeably lower activities. This highlights the importance of the role played by the NHO in the activity of the catalyst. Moreover, by reacting the IrPCP(NHO) catalyst with an excess of HCOOH and pyridine we were able to isolate a plausible reaction intermediate. These postulations have been substantiated by DFT calculations.

Idioma: Inglés

DOI: 10.1039/c8gc02794c

Año: 2018

Publicado en: GREEN CHEMISTRY 20, 21 (2018), 4875-4879
ISSN: 1463-9262

Factor impacto JCR: 9.405 (2018)

Categ. JCR: GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY rank: 2 / 35 = 0.057 (2018) - Q1 - T1
Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 20 / 172 = 0.116 (2018) - Q1 - T1

Factor impacto SCIMAGO: 2.517 - Pollution (Q1) - Environmental Chemistry (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA-FSE/E42-17R
Financiación: info:eu-repo/grantAgreement/ES/MECD/FPU14-06003
Financiación: info:eu-repo/grantAgreement/ES/MICINN-FEDER/CTQ2016-75884-P
Financiación: info:eu-repo/grantAgreement/ES/MICINN/RYC-2016-20864

Tipo y forma: Artículo (PostPrint)

Área (Departamento): Área Química Inorgánica (Dpto. Química Inorgánica)
Área (Departamento): Área Química Física (Dpto. Química Física)