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Artificial metalloenzymes as catalysts for oxidative lignin degradation

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dc.contributor.authorDoble, Megan
dc.contributor.authorJarvis, Amanda
dc.contributor.authorWard, Andy
dc.contributor.authorColburn, Jonathan David
dc.contributor.authorGoetze, Jan Philipp
dc.contributor.authorBuehl, Michael
dc.contributor.authorKamer, Paul C J
dc.date.accessioned2019-10-09T23:37:20Z
dc.date.available2019-10-09T23:37:20Z
dc.date.issued2018-11-05
dc.identifier256176559
dc.identifiercbbe6e9a-2f50-473f-b26d-d5385e12bd2f
dc.identifier85056253697
dc.identifier000449577200162
dc.identifier.citationDoble , M , Jarvis , A , Ward , A , Colburn , J D , Goetze , J P , Buehl , M & Kamer , P C J 2018 , ' Artificial metalloenzymes as catalysts for oxidative lignin degradation ' , ACS Sustainable Chemistry & Engineering , vol. 6 , no. 11 , pp. 15100-15107 . https://doi.org/10.1021/acssuschemeng.8b03568en
dc.identifier.issn2168-0485
dc.identifier.otherORCID: /0000-0002-1095-7143/work/49308208
dc.identifier.urihttps://hdl.handle.net/10023/18635
dc.descriptionM.V.D thanks the BBSRC for support through an EastBio studentship BB/J01446X/1. The authors thank the EPSRC for funding through the EPSRC critical mass grant “Clean catalysis for sustainable development” (EP/J018139/1). This work was supported by the EU the European Union (Marie Curie ITN “SuBiCat” PITN-GA-2013-60704 (P.C.J.K), and through a Marie Curie Individual Fellowship project ArtOxiZymes to A.G.J. (H2020-MSCA-IF-2014- 657755). A.G.J would also like to thank the University of Edinburgh for funding through a Christina Miller Fellowship. The UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium, which is funded by the EPSRC (EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1, and EP/M013219/1).en
dc.description.abstractWe report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme.
dc.format.extent8
dc.format.extent1314276
dc.language.isoeng
dc.relation.ispartofACS Sustainable Chemistry & Engineeringen
dc.subjectLigninen
dc.subjectArtificial metalloenzymesen
dc.subjectCatalytic oxidationen
dc.subjectQD Chemistryen
dc.subjectDASen
dc.subject.lccQDen
dc.titleArtificial metalloenzymes as catalysts for oxidative lignin degradationen
dc.typeJournal articleen
dc.contributor.sponsorEPSRCen
dc.contributor.sponsorEPSRCen
dc.contributor.sponsorMarie Curie Fellowshipsen
dc.contributor.sponsorEuropean Commissionen
dc.contributor.institutionUniversity of St Andrews. School of Chemistryen
dc.contributor.institutionUniversity of St Andrews. EaSTCHEMen
dc.identifier.doi10.1021/acssuschemeng.8b03568
dc.description.statusPeer revieweden
dc.date.embargoedUntil2019-10-10
dc.identifier.grantnumberEP/J018139/1en
dc.identifier.grantnumberEP/J018139/1en
dc.identifier.grantnumberSUBICATen
dc.identifier.grantnumber657755en


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