Unbiased Photoelectrode Interfaces for Solar Coupling of Lignin Oxidation with Biocatalytic C=C Bond Hydrogenation

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dc.contributor.authorKim, Jinhyunko
dc.contributor.authorUm, Yunnako
dc.contributor.authorHan, Seunghyunko
dc.contributor.authorHilberath, Thomasko
dc.contributor.authorKim, Yong Hwanko
dc.contributor.authorHollmann, Frankko
dc.contributor.authorPark, Chan Beumko
dc.date.accessioned2022-05-09T03:01:42Z-
dc.date.available2022-05-09T03:01:42Z-
dc.date.created2022-05-09-
dc.date.created2022-05-09-
dc.date.issued2022-03-
dc.identifier.citationACS APPLIED MATERIALS & INTERFACES, v.14, no.9, pp.11465 - 11473-
dc.identifier.issn1944-8244-
dc.identifier.urihttp://hdl.handle.net/10203/296460-
dc.description.abstractThe pulp and paper manufacturers generate approximately 50 million metric tons of lignin per annum, most of which has been abandoned or incinerated because of lignin's recalcitrant nature. Here, we report bias-free photoelectrochemical (PEC) oxidation of lignin coupled with asymmetric hydrogenation of C=C bonds. The PEC platform consists of a hematite (alpha-Fe2O3) photoanode and a silicon photovoltaic-wired mesoporous indium tin oxide (Si/mesoITO) photocathode. We substantiate a new function of photoelectroactivated alpha-Fe2O3 to extract electrons from lignin. The extracted electrons are transferred to the Si/mesoITO photocathode for regenerating synthetic nicotinamide cofactor analogues (mNADHs). We demonstrate that the reduction kinetics of mNAD(+)s depend on their reduction peak potentials. The regenerated mNADHs activate ene-reductases from the old yellow enzyme (OYE) family, which catalyze enantioselective reduction of alpha,beta-unsaturated hydrocarbons. This lignin-fueled biocatalytic PEC system exhibits an excellent OYE's turnover frequency and total turnover number for photobiocatalytic trans-hydrogenation through cofactor regeneration. This work presents the first example of PEC regeneration of mNADHs and opens up a sustainable route for bias-free chemical synthesis using renewable lignin waste as an electron feedstock.-
dc.languageEnglish-
dc.publisherAMER CHEMICAL SOC-
dc.titleUnbiased Photoelectrode Interfaces for Solar Coupling of Lignin Oxidation with Biocatalytic C=C Bond Hydrogenation-
dc.typeArticle-
dc.identifier.wosid000787543300038-
dc.identifier.scopusid2-s2.0-85125933497-
dc.type.rimsART-
dc.citation.volume14-
dc.citation.issue9-
dc.citation.beginningpage11465-
dc.citation.endingpage11473-
dc.citation.publicationnameACS APPLIED MATERIALS & INTERFACES-
dc.identifier.doi10.1021/acsami.1c24342-
dc.contributor.localauthorPark, Chan Beum-
dc.contributor.nonIdAuthorUm, Yunna-
dc.contributor.nonIdAuthorHan, Seunghyun-
dc.contributor.nonIdAuthorHilberath, Thomas-
dc.contributor.nonIdAuthorKim, Yong Hwan-
dc.contributor.nonIdAuthorHollmann, Frank-
dc.description.isOpenAccessN-
dc.type.journalArticleArticle-
dc.subject.keywordAuthorlignin-
dc.subject.keywordAuthorhematite-
dc.subject.keywordAuthorphotoelectrocatalysis-
dc.subject.keywordAuthorbiocatalysis-
dc.subject.keywordAuthortrans-hydrogenation-
dc.subject.keywordPlusNICOTINAMIDE-
dc.subject.keywordPlusCHEMICALS-
dc.subject.keywordPlusLIGHT-
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