Sequence Rules the Functional Connections and Efficiency of Catalytic Precision Oligomers

Jie Li; Qian Qin; Sinan Kardas; Mathieu Fossépré; Mathieu Surin; Antony E. Fernandes; Karine Glinel; Alain M. Jonas

doi:10.1021/acscatal.1c05560

Sequence Rules the Functional Connections and Efficiency of Catalytic Precision Oligomers

Jie Li
, Qian Qin
, Sinan Kardas
, Mathieu Fossépré
, Mathieu Surin (Corresponding author)
, Antony E. Fernandes
, Karine Glinel
, Alain M. Jonas (Corresponding author)

Onderzoeksoutput: Bijdrage aan tijdschrift › Tijdschriftartikel › Academic › peer review

15 Citaten (Scopus)

142 Downloads (Pure)

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The efficiency of cooperative catalysts is dependent on the probabilities of chance encounter between the different complementary catalytic units. Connecting these catalytic groups along a short flexible oligomeric chain increases these probabilities. Here, we show that the sequence of a catalytic triad precisely positioned along a flexible backbone also strongly matters, with the catalytic activity varying by up to 1 order of magnitude when interchanging two groups in the oligomer sequence. These results are rationalized with molecular graphs computed from molecular dynamics simulations, showing how functional connections between catalytic groups are dependent on sequence order.

Originele taal-2	Engels
Pagina's (van-tot)	2126-2131
Aantal pagina's	6
Tijdschrift	ACS Catalysis
Volume	12
Nummer van het tijdschrift	3
DOI's	https://doi.org/10.1021/acscatal.1c05560
Status	Gepubliceerd - 4 feb. 2022

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The authors acknowledge the Fonds de la Recherche Scientifique - FNRS and the Fonds Wetenschappelijk Onderzoek, under EOS Project No. 30650939 for financial support. Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by FNRS (Grant No. 2.5020.11) and Wallonia Region. The authors acknowledge Gabriella Barrozino-Consiglio for 500 MHz NMR analysis, Raoul Rozenberg for APCI-MS, Hervé Degand for ESI-MS/MS analysis, and Laurent Collard for GC analysis. K.G. and M.S. are Senior Research Associates of the F.R.S.–FNRS.

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title = "Sequence Rules the Functional Connections and Efficiency of Catalytic Precision Oligomers",

abstract = "The efficiency of cooperative catalysts is dependent on the probabilities of chance encounter between the different complementary catalytic units. Connecting these catalytic groups along a short flexible oligomeric chain increases these probabilities. Here, we show that the sequence of a catalytic triad precisely positioned along a flexible backbone also strongly matters, with the catalytic activity varying by up to 1 order of magnitude when interchanging two groups in the oligomer sequence. These results are rationalized with molecular graphs computed from molecular dynamics simulations, showing how functional connections between catalytic groups are dependent on sequence order. ",

keywords = "aerobic oxidation, alcohols, graph theory, Multifunctional catalysis, precision oligomers",

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note = "Funding Information: The authors acknowledge the Fonds de la Recherche Scientifique - FNRS and the Fonds Wetenschappelijk Onderzoek, under EOS Project No. 30650939 for financial support. Computational resources have been provided by the Consortium des {\'E}quipements de Calcul Intensif (C{\'E}CI), funded by FNRS (Grant No. 2.5020.11) and Wallonia Region. The authors acknowledge Gabriella Barrozino-Consiglio for 500 MHz NMR analysis, Raoul Rozenberg for APCI-MS, Herv{\'e} Degand for ESI-MS/MS analysis, and Laurent Collard for GC analysis. K.G. and M.S. are Senior Research Associates of the F.R.S.–FNRS. ",

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AU - Surin, Mathieu

AU - Fernandes, Antony E.

AU - Glinel, Karine

AU - Jonas, Alain M.

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AB - The efficiency of cooperative catalysts is dependent on the probabilities of chance encounter between the different complementary catalytic units. Connecting these catalytic groups along a short flexible oligomeric chain increases these probabilities. Here, we show that the sequence of a catalytic triad precisely positioned along a flexible backbone also strongly matters, with the catalytic activity varying by up to 1 order of magnitude when interchanging two groups in the oligomer sequence. These results are rationalized with molecular graphs computed from molecular dynamics simulations, showing how functional connections between catalytic groups are dependent on sequence order.

KW - aerobic oxidation

KW - alcohols

KW - graph theory

KW - Multifunctional catalysis

KW - precision oligomers

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Sequence Rules the Functional Connections and Efficiency of Catalytic Precision Oligomers

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