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001031817 1001_ $$0P:(DE-Juel1)178762$$aJäckering, Anna$$b0
001031817 245__ $$aInfluence of Wobbling Tryptophan and Mutations on PET Degradation Explored by QM/MM Free Energy Calculations
001031817 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2024
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001031817 520__ $$aABSTRACT: Plastic-degrading enzymes, particularly poly(ethylene terephthalate)(PET) hydrolases, have garnered significant attention in recent years aspotential eco-friendly solutions for recycling plastic waste. However, understandingof their PET-degrading activity and influencing factors remainsincomplete, impeding the development of uniform approaches for enhancingPET hydrolases for industrial applications. A key aspect of PET hydrolaseengineering is optimizing the PET-hydrolysis reaction by lowering the associatedfree energy barrier. However, inconsistent findings have complicated these efforts.Therefore, our goal is to elucidate various aspects of enzymatic PET degradationby means of quantum mechanics/molecular mechanics (QM/MM) reactionsimulations and analysis, focusing on the initial reaction step, acylation, in twothermophilic PET hydrolases, LCC and PES-H1, along with their highly active variants, LCCIG and PES-H1FY. Our findingshighlight the impact of semiempirical QM methods on proton transfer energies, affecting the distinction between a two-step reactioninvolving a metastable tetrahedral intermediate and a one-step reaction. Moreover, we uncovered a concerted conformational changeinvolving the orientation of the PET benzene ring, altering its interaction with the side-chain of the “wobbling” tryptophan from Tstackingto parallel π−π interactions, a phenomenon overlooked in prior research. Our study thus enhances the understanding of theacylation mechanism of PET hydrolases, in particular by characterizing it for the first time for the promising PES-H1FY using QM/MM simulations. It also provides insights into selecting a suitable QM method and a reaction coordinate, valuable for future studieson PET degradation processes.
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001031817 7001_ $$0P:(DE-HGF)0$$avan der Kamp, Marc$$b1
001031817 7001_ $$0P:(DE-Juel1)132024$$aStrodel, Birgit$$b2$$eCorresponding author
001031817 7001_ $$0P:(DE-HGF)0$$aZinovjev, Kirill$$b3
001031817 770__ $$aApplications of Free-Energy Calculations to Biomolecular Processes
001031817 773__ $$0PERI:(DE-600)1491237-5$$a10.1021/acs.jcim.4c00776$$gp. acs.jcim.4c00776$$pacs.jcim.4c00776$$tJournal of chemical information and modeling$$v11$$x1549-9596$$y2024
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