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oai:recercat.cat:10256/181812024-10-29T23:14:59Zcom_2072_452955com_2072_2054col_2072_453073

Intrinsic enzymatic properties modulate the self-propulsion of micromotors Arqué, Xavier Romero Rivera, Adrian Feixas Geronès, Ferran Patiño, Tania Osuna Oliveras, Sílvia Sánchez, Samuel Cinètica enzimàtica Enzyme kinetics Catàlisi Catalysis Bio-catalytic micro- and nanomotors self-propel by the enzymatic conversion of substrates into products. Despite the advances in the field, the fundamental aspects underlying enzymepowered self-propulsion have rarely been studied. In this work, we select four enzymes (urease, acetylcholinesterase, glucose oxidase, and aldolase) to be attached on silica microcapsules and study how their turnover number and conformational dynamics affect the self-propulsion, combining both an experimental and molecular dynamics simulations approach. Urease and acetylcholinesterase, the enzymes with higher catalytic rates, are the only enzymes capable of producing active motion. Molecular dynamics simulations reveal that urease and acetylcholinesterase display the highest degree of flexibility near the active site, which could play a role on the catalytic process. We experimentally assess this hypothesis for urease micromotors through competitive inhibition (acetohydroxamic acid) and increasing enzyme rigidity (β-mercaptoethanol). We conclude that the conformational changes are a precondition of urease catalysis, which is essential to generate self-propulsio The research leading to these results has received funding from the Spanish MINECO for grants CTQ2015-68879-R (MICRODIA) and CTQ2015-72471-EXP (Enzwim). T.P. thanks MINECO for the Juan de la Cierva fellowship (FJCI-2015-25578). A.R.-R. thanks the Generalitat de Catalunya for PhD fellowship (2015-FI-B-00165). F.F. thanks the European Community for MSCA-IF-2014-EF-661160-MetAccembly grant. S.O. thanks funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (ERC-2015-StG-679001). F.F., A.R.-R., and S.O. thank the Generalitat de Catalunya for grup emergent 2017 SGR-1707. S.S. acknowledges Foundation BBVA for the MEDIROBOTS project and the CERCA program by the Generalitat de Catalunya 2019-06-27 info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion peer-reviewed info:eu-repo/semantics/altIdentifier/doi/10.1038/s41467-019-10726-8 info:eu-repo/semantics/altIdentifier/issn/2041-1723 info:eu-repo/grantAgreement/EC/H2020/661160/EU/Accelerating metal-directed assembly, recognition and catalysis with computational methods/MetAccembly Attribution 4.0 International http://creativecommons.org/licenses/by/4.0/ info:eu-repo/semantics/openAccess Nature Research Nature Communications, 2019, vol. 10, art. núm. 2826 Articles publicats (D-Q)