000131818 001__ 131818
000131818 005__ 20241125101202.0
000131818 0247_ $$2doi$$a10.1021/acssuschemeng.3c02958
000131818 0248_ $$2sideral$$a137222
000131818 037__ $$aART-2023-137222
000131818 041__ $$aeng
000131818 100__ $$aDiamanti, Eleftheria
000131818 245__ $$aSelf-Sufficient Heterogeneous Biocatalysis through Boronic Acid-Diol Complexation of Adenylated Cofactors
000131818 260__ $$c2023
000131818 5060_ $$aAccess copy available to the general public$$fUnrestricted
000131818 5203_ $$aSelf-sufficient heterogeneous biocatalysts (ssHB) are promising candidates for implementing cofactor-dependent enzymes in chemical biomanufacturing. Most strategies for coimmobilizing cofactors with dehydrogenases on porous agarose microbeads involve the use of cationic polymers (i.e., polyethylenimine, PEI) that interact electrostatically with the phosphate groups of their corresponding phosphorylated cofactors. Although the latter is a powerful and versatile approach, ionic bonds are disrupted in biotransformations operating at a high ionic strength, where screening of bonded ions takes place. Harnessing the ribose groups present in adenylated cofactors, we immobilize a selection of these (NAD(P)H, NAD(P)+, FAD, and ATP) on agarose microbeads functionalized with boronic acid to establish reversible covalent bonds between the cis-diol of the ribose in the cofactor backbone and the boronic acid. To do so, we functionalize cobalt-activated porous agarose beads with boronic acid (AG-B/Co2+) for the coimmobilization of adenylated cofactors with the corresponding cofactor dependent His-tagged dehydrogenases. First, we demonstrate that the adenylated cofactor-support interactions are reversible but show resistance against high salt concentrations, overcoming the main limitation of the current self-sufficient heterogeneous biocatalysts. Then, we coimmobilized several His-tagged enzymes with their corresponding adenylated cofactors and investigated the functionality and stability of these ssHBs in reductive aminations performed under high ionic strength in both batch and flow reactors. As a result, we manage to reuse the immobilized enzymes and the cofactors 3.5 × 105 and 167 times, respectively. This work expands the usefulness of ssBHs for hitherto bioprocess regardless of the ionic strength of the media.
000131818 536__ $$9info:eu-repo/grantAgreement/EC/H2020/818089/EU/Artificial metabolic cells for biomanufacturing of bio-based chiral fine chemicals/METACELL$$9This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 818089-METACELL$$9info:eu-repo/grantAgreement/ES/MICINN/MDM-2017-0720
000131818 540__ $$9info:eu-repo/semantics/openAccess$$aAll rights reserved$$uhttp://www.europeana.eu/rights/rr-f/
000131818 590__ $$a7.1$$b2023
000131818 592__ $$a1.664$$b2023
000131818 591__ $$aENGINEERING, CHEMICAL$$b21 / 170 = 0.124$$c2023$$dQ1$$eT1
000131818 591__ $$aGREEN & SUSTAINABLE SCIENCE & TECHNOLOGY$$b21 / 91 = 0.231$$c2023$$dQ1$$eT1
000131818 591__ $$aCHEMISTRY, MULTIDISCIPLINARY$$b43 / 231 = 0.186$$c2023$$dQ1$$eT1
000131818 593__ $$aEnvironmental Chemistry$$c2023$$dQ1
000131818 593__ $$aRenewable Energy, Sustainability and the Environment$$c2023$$dQ1
000131818 593__ $$aChemistry (miscellaneous)$$c2023$$dQ1
000131818 593__ $$aChemical Engineering (miscellaneous)$$c2023$$dQ1
000131818 594__ $$a13.8$$b2023
000131818 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/acceptedVersion
000131818 700__ $$0(orcid)0000-0001-9478-6750$$aVelasco-Lozano, Susana
000131818 700__ $$aGrajales-Hernández, Daniel
000131818 700__ $$aOrrego, Alejandro H.
000131818 700__ $$aDi Silvio, Desiré
000131818 700__ $$0(orcid)0000-0002-0136-5138$$aFraile, José María
000131818 700__ $$aLópez-Gallego, Fernando
000131818 773__ $$g11, 39 (2023), 14409-14421$$pACS sustain. chem. & eng.$$tACS Sustainable Chemistry and Engineering$$x2168-0485
000131818 8564_ $$s858920$$uhttps://zaguan.unizar.es/record/131818/files/texto_completo.pdf$$yPostprint$$zinfo:eu-repo/date/embargoEnd/2024-09-21
000131818 8564_ $$s2625931$$uhttps://zaguan.unizar.es/record/131818/files/texto_completo.jpg?subformat=icon$$xicon$$yPostprint$$zinfo:eu-repo/date/embargoEnd/2024-09-21
000131818 909CO $$ooai:zaguan.unizar.es:131818$$particulos$$pdriver
000131818 951__ $$a2024-11-22-12:12:27
000131818 980__ $$aARTICLE