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Analysis of institutional authors

Kqiku, LauraAuthorSchiel, FlorianAuthor

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October 22, 2024
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Article

Stereospecific radical coupling with a non-natural photodecarboxylase

Publicated to: Nature. 634 (8035): - 2024-10-24 634(8035), DOI: 10.1038/s41586-024-08004-9

Authors:

Tseliou, V; Kqiku, L; Berger, M; Schiel, F; Zhou, HY; Poelarends, GJ; Melchiorre, P
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Affiliations

Barcelona Inst Sci & Technol, Inst Chem Res Catalonia, ICIQ, Tarragona, Spain - Author
Univ Bologna, Dept Ind Chem Toso Montanari, Bologna, Italy - Author
Univ Groningen, Groningen Res Inst Pharm, Dept Chem & Pharmaceut Biol, Groningen, Netherlands - Author
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Abstract

Photoenzymes are light-powered biocatalysts that typically rely on the excitation of cofactors or unnatural amino acids for their catalytic activities1,2. A notable natural example is the fatty acid photodecarboxylase, which uses light energy to convert aliphatic carboxylic acids to achiral hydrocarbons3. Here we report a method for the design of a non-natural photodecarboxylase based on the excitation of enzyme-bound catalytic intermediates, rather than reliance on cofactor excitation4. Iminium ions5, transiently generated from enals within the active site of an engineered class I aldolase6, can absorb violet light and function as single-electron oxidants. Activation of chiral carboxylic acids, followed by decarboxylation, generates two radicals that undergo stereospecific cross-coupling, yielding products with two stereocentres. Using the appropriate enantiopure chiral substrate, the desired diastereoisomeric product is selectively obtained with complete enantiocontrol. This finding underscores the ability of the active site to transfer stereochemical information from the chiral radical precursor into the product, effectively addressing the long-standing problem of rapid racemization of chiral radicals. The resulting 'memory of chirality' scenario7 is a rarity in enantioselective radical chemistry. We report a method for the design of a non-natural photodecarboxylase based on the excitation of enzyme-bound catalytic intermediates, rather than reliance on cofactor excitation.
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Keywords

AcidsChiralityEnableMechanismsMemoryStrategies

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal NATURE due to its progression and the good impact it has achieved in recent years, according to the agency WoS (JCR), it has become a reference in its field. In the year of publication of the work, 2024 there are still no calculated indicators, but in 2023, it was in position 2/136, thus managing to position itself as a Q1 (Primer Cuartil), in the category Multidisciplinary Sciences. Notably, the journal is positioned above the 90th percentile.

Independientemente del impacto esperado determinado por el canal de difusión, es importante destacar el impacto real observado de la propia aportación.

Según las diferentes agencias de indexación, el número de citas acumuladas por esta publicación hasta la fecha 2026-04-04:

  • WoS: 39
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Impact and social visibility

From the perspective of influence or social adoption, and based on metrics associated with mentions and interactions provided by agencies specializing in calculating the so-called "Alternative or Social Metrics," we can highlight as of 2026-04-04:

  • The use, from an academic perspective evidenced by the Altmetric agency indicator referring to aggregations made by the personal bibliographic manager Mendeley, gives us a total of: 57.
  • The use of this contribution in bookmarks, code forks, additions to favorite lists for recurrent reading, as well as general views, indicates that someone is using the publication as a basis for their current work. This may be a notable indicator of future more formal and academic citations. This claim is supported by the result of the "Capture" indicator, which yields a total of: 48 (PlumX).

With a more dissemination-oriented intent and targeting more general audiences, we can observe other more global scores such as:

  • The Total Score from Altmetric: 71.
  • The number of mentions on the social network X (formerly Twitter): 54 (Altmetric).
  • The number of mentions in news outlets: 4 (Altmetric).

It is essential to present evidence supporting full alignment with institutional principles and guidelines on Open Science and the Conservation and Dissemination of Intellectual Heritage. A clear example of this is:

  • The work has been submitted to a journal whose editorial policy allows open Open Access publication.
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Leadership analysis of institutional authors

This work has been carried out with international collaboration, specifically with researchers from: Italy; Netherlands.

There is a significant leadership presence as some of the institution’s authors appear as the first or last signer, detailed as follows: First Author (Tseliou, Vasilis) .

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Awards linked to the item

We thank W. Hartley for fruitful discussions; M. Haring for assistance with the synthesis of reference compounds; E. C. Escudero Adan, M. Martinez and J. Benet for X-ray crystallographic analysis; X. Caldentey for assistance with high-throughput screening studies; and N. Cabello Sanchez for assistance with mass spectrometry analysis. Financial support was provided by the ICIQ 'Strategic Funds Call 2021', Project PRINPNRR 'LIGHT CAT' (no. P2022RHMCM) supported by the European Commission - NextGeneration EU programme - M4C2 and Agencia Estatal de Investigacion (no. PID2019-106278GB-I00). V.T. thanks the European Union for a Horizon 2020 Marie Sklodowska-Curie Fellowship (no. H2020-MSCA-IF-2020101032077). L.K. thanks MCIN/AEI/10.13039/501100011033 and ESF for a predoctoral grant (no. PRE2020-095712). M.B. thanks the Austrian Science Fund (FWF, no. J4603-N) for an Erwin-Schroedinger postdoctoral fellowship. H.Z. acknowledges funding from the China Scholarship Council (no. CSC202008420244).
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