Building lactams by highly selective hydrodeoxygenation of cyclic imides using an alumina-supported AgRe bimetallic nanocatalyst
The rational design of robust nanocatalysts containing the suitable active sites for building relevant organic compounds, such as lactams, is a desired approximation towards the development of a sustainable fine chemistry field. In that sense, the design of a proper nanomaterial able to mediate the selective hydrodeoxygenation of cyclic imides to lactams with high tolerance to the preservation of aromatic rings remains rather unexplored. Here, we show the design of a bimetallic AgRe nanomaterial with notable activity and selectivity to mediate this transformation affording more than 60 lactams from the corresponding imides. Interestingly, in this work we disclose that the optimal AgRe nanocatalyst is constituted by AgReO<sub>4</sub> nanoaggregates that undergo an in situ hydrogenative dispersion to form the active centers composed by Ag<sup>0</sup> nanoparticles and ReO<sub>x</sub> species. Deep characterization, together with kinetic and mechanistic studies, have revealed that the intimate Ag-Re contact intrinsic to AgReO<sub>4</sub> species is key for the formation of the most active catalytic sites and the proper bimetallic cooperation required for mediating the desired process.
Authors
- Laura Simonelli (ORCID: https://orcid.org/0000-0001-5331-0633)
- Rosa Adam (ORCID: https://orcid.org/0000-0001-9392-7187)
- Juan Camilo Arango‐Daza (ORCID: https://orcid.org/0000-0002-8209-0622)
- Carles Lluna‐Galán (ORCID: https://orcid.org/0000-0003-1761-9275)
- José J. Calvino (ORCID: https://orcid.org/0000-0002-0989-1335)
- Patricia Concepción (ORCID: https://orcid.org/0000-0003-2058-3103)
- Rong Sun (ORCID: https://orcid.org/0000-0002-9252-5132)
- Jose R. Cabrero‐Antonino (ORCID: https://orcid.org/0000-0001-9628-9803)
- Daviel Gómez (ORCID: https://orcid.org/0000-0003-0010-4507)
Institutions
- Universitat de València (ES)
- ALBA Synchrotron (Spain) (ES)
- Universidad de Cádiz (ES)
- Instituto de Tecnología Química (ES)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-05-02
- DOI
- https://doi.org/10.1038/s41467-025-59514-7
- Citations
- 6
- Primary Topic
- Asymmetric Hydrogenation and Catalysis
- Type
- article
- Field-Weighted Citation Impact
- 3.22
Funders
- European Commission
- Generalitat Valenciana
- Ministerio de Ciencia e Innovación
- Fundación Bancaria Caixa d'Estalvis i Pensions de Barcelona
- Agencia Estatal de Investigación