000151279 001__ 151279
000151279 005__ 20251017144611.0
000151279 0247_ $$2doi$$a10.1039/d1ob00305d
000151279 0248_ $$2sideral$$a124086
000151279 037__ $$aART-2021-124086
000151279 041__ $$aeng
000151279 100__ $$aGarcia-Sanz, C.
000151279 245__ $$aPd-Oxazolone complexes conjugated to an engineered enzyme: improving fluorescence and catalytic properties
000151279 260__ $$c2021
000151279 5060_ $$aAccess copy available to the general public$$fUnrestricted
000151279 5203_ $$aDifferent Pd-complexes containing orthometallated push-pull oxazolones were inserted by supramolecular Pd-amino acid coordination on two genetically engineered modified variants of the thermoalkalophilicGeobacillus thermocatenolatuslipase (GTL). Pd-lipase conjugation was performed on the solid phase in the previously immobilized form of GTL under mild conditions, and soluble conjugated Pd-GTL complexes were obtained by simply desorbing by washing with an acetonitrile aqueous solution. Three different Pd complexes were incorporated into two different genetically modified enzyme variants, one containing all the natural cysteine residues changed to serine residues, and another variant including an additional Cys mutation directly in the catalytic serine (Ser114Cys). The new Pd-enzyme conjugates were fluorescent even at ppm concentrations, while under the same conditions free Pd complexes did not show fluorescence at all. The Pd conjugation with the enzyme extremely increases the catalytic profile of the corresponding Pd complex from 200 to almost 1000-fold in the hydrogenation of arenes in aqueous media, achieving in the case of GTL conjugated with orthopalladated4aan outstanding TOF value of 27¿428 min-1. Also the applicability of GTL-C114 conjugated with orthopalladated4bin a site-selective C-H activation reaction under mild conditions has been demonstrated. Therefore, the Pd incorporation into the enzyme produces a highly stable conjugate, and improves remarkably the catalytic activity and selectivity, as well as the fluorescence intensity, of the Pd complexes.
000151279 536__ $$9info:eu-repo/grantAgreement/EUR/COST/CA15106-CHAOS$$9info:eu-repo/grantAgreement/ES/DGA/E19-20R$$9info:eu-repo/grantAgreement/ES/DGA-FEDER/LMP144-18$$9info:eu-repo/grantAgreement/ES/MICINN/AGL2017-84614-C2-2-R$$9info:eu-repo/grantAgreement/ES/MICINN/PID2019-106394GB-I00
000151279 540__ $$9info:eu-repo/semantics/openAccess$$aby-nc$$uhttps://creativecommons.org/licenses/by-nc/4.0/deed.es
000151279 590__ $$a3.89$$b2021
000151279 591__ $$aCHEMISTRY, ORGANIC$$b13 / 56 = 0.232$$c2021$$dQ1$$eT1
000151279 592__ $$a0.832$$b2021
000151279 593__ $$aPhysical and Theoretical Chemistry$$c2021$$dQ1
000151279 593__ $$aOrganic Chemistry$$c2021$$dQ1
000151279 594__ $$a6.5$$b2021
000151279 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/publishedVersion
000151279 700__ $$aAndreu, A.
000151279 700__ $$ade las Rivas, B.
000151279 700__ $$0(orcid)0000-0001-8057-4861$$aJimenez, A.I.
000151279 700__ $$aPop, A.
000151279 700__ $$aSilvestru, C.
000151279 700__ $$0(orcid)0000-0001-9779-5820$$aUrriolabeitia, E.P.
000151279 700__ $$aPalomo, J.M.
000151279 773__ $$g19, 12 (2021), 2773-2783$$pOrg. biomol. chem.$$tOrganic & Biomolecular Chemistry$$x1477-0520
000151279 8564_ $$s1590424$$uhttps://zaguan.unizar.es/record/151279/files/texto_completo.pdf$$yVersión publicada
000151279 8564_ $$s2705619$$uhttps://zaguan.unizar.es/record/151279/files/texto_completo.jpg?subformat=icon$$xicon$$yVersión publicada
000151279 909CO $$ooai:zaguan.unizar.es:151279$$particulos$$pdriver
000151279 951__ $$a2025-10-17-14:17:16
000151279 980__ $$aARTICLE