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.

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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

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article

Building lactams by highly selective hydrodeoxygenation of cyclic imides using an alumina-supported AgRe bimetallic nanocatalyst

Laura Simonelli, Rosa Adam, Juan Camilo Arango‐Daza, Carles Lluna‐Galán et al.
6 citations
Nature Communications
Asymmetric Hydrogenation and Catalysis
3.22
article

Building lactams by highly selective hydrodeoxygenation of cyclic imides using an alumina-supported AgRe bimetallic nanocatalyst

Laura Simonelli, Rosa Adam, Juan Camilo Arango‐Daza, Carles Lluna‐Galán, José J. Calvino, Patricia Concepción, Rong Sun, Jose R. Cabrero‐Antonino, Daviel Gómez
article en
6 citations

Abstract

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.

Nature CommunicationsVol. 16(1)
Universitat de València (ES), ALBA Synchrotron (Spain) (ES), Universidad de Cádiz (ES), Instituto de Tecnología Química (ES)
European Commission, Generalitat Valenciana, Ministerio de Ciencia e Innovación, Fundación Bancaria Caixa d'Estalvis i Pensions de Barcelona, Agencia Estatal de Investigación
Openalex Percentile: Top 8%
Asymmetric Hydrogenation and Catalysis
3.22
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