Piezobiocatalysis: Ultrasound-Driven Enzymatic Oxyfunctionalization of C-H Bonds

Cited 3 time in webofscience Cited 0 time in scopus
  • Hit : 94
  • Download : 0
DC FieldValueLanguage
dc.contributor.authorYoon, Jaehoko
dc.contributor.authorKim, Jinhyunko
dc.contributor.authorTieves, Florianko
dc.contributor.authorZhang, Wuyuanko
dc.contributor.authorAlcalde, Miguelko
dc.contributor.authorHollmann, Frankko
dc.contributor.authorPark, Chan Beumko
dc.date.accessioned2020-05-27T01:20:14Z-
dc.date.available2020-05-27T01:20:14Z-
dc.date.created2020-05-25-
dc.date.created2020-05-25-
dc.date.created2020-05-25-
dc.date.issued2020-05-
dc.identifier.citationACS CATALYSIS, v.10, no.9, pp.5236 - 5242-
dc.identifier.issn2155-5435-
dc.identifier.urihttp://hdl.handle.net/10203/274315-
dc.description.abstractPeroxygenases have long inspired the selective oxyfunctionalization of various aliphatic and aromatic compounds, because of their broad substrate spectrum and simplicity of catalytic mechanism. This study provides a proof-of-concept of piezobiocatalysis by demonstrating peroxygenase-catalyzed oxyfunctionalization reactions fueled by piezocatalytically generated H2O2. Bismuth oxychloride (BiOCl) generated H2O2 in situ via an oxygen reduction reaction under ultrasonic wave conditions. Through the simple combination of water, ultrasound, recombinant, evolved unspecific peroxygenase from Agrocybe aegerita (rAaeUPO), and BiOCl, the piezobiocatalytic platform accelerated selective hydroxylation of ethylbenzene to enantiopure (R)-1-phenylethanol [total turnover number of rAaeUPO (TTNrAaeUPO), 2002; turnover frequency, 77.7 min(-1); >99% enantiomeric excess (ee)]. The BiOCl-rAaeUPO couple also catalyzed other representative substrates (e.g., propylbenzene, 1-chloro-4-ethylbenzene, cyclohexane, and cis-beta-methylstyrene) with high turnover frequency and selectivity. We alleviated the oxidative stress of piezocatalytically generated OH center dot on rAaeUPO by spatial separation of rAaeUPO and BiOCl, which resulted in greatly enhanced TTNrAaeUPO of >3900 and the notable prolongation of reaction time. Overall, the BiOCl-rAaeUPO couple serves as a mechanical-to-chemical energy conversion platform for driving peroxygenase-catalyzed reactions under ultrasonic conditions.-
dc.languageEnglish-
dc.publisherAMER CHEMICAL SOC-
dc.titlePiezobiocatalysis: Ultrasound-Driven Enzymatic Oxyfunctionalization of C-H Bonds-
dc.typeArticle-
dc.identifier.wosid000530090800043-
dc.type.rimsART-
dc.citation.volume10-
dc.citation.issue9-
dc.citation.beginningpage5236-
dc.citation.endingpage5242-
dc.citation.publicationnameACS CATALYSIS-
dc.identifier.doi10.1021/acscatal.0c00188-
dc.contributor.localauthorPark, Chan Beum-
dc.contributor.nonIdAuthorTieves, Florian-
dc.contributor.nonIdAuthorZhang, Wuyuan-
dc.contributor.nonIdAuthorAlcalde, Miguel-
dc.contributor.nonIdAuthorHollmann, Frank-
dc.description.isOpenAccessN-
dc.type.journalArticleArticle-
dc.subject.keywordAuthoroxidation-
dc.subject.keywordAuthoroxyfunctionalization-
dc.subject.keywordAuthorperoxygenase-
dc.subject.keywordAuthorpiezocatalysis-
dc.subject.keywordAuthorpiezobiocatalysis-
dc.subject.keywordPlusPHOTOCATALYTIC ACTIVITY-
dc.subject.keywordPlusAEROBIC OXIDATION-
dc.subject.keywordPlusSOLAR-DRIVEN-
dc.subject.keywordPlusOXYGEN-
dc.subject.keywordPlusPEROXYGENASES-
dc.subject.keywordPlusNANOSHEETS-
dc.subject.keywordPlusCHALLENGE-
dc.subject.keywordPlusMECHANISM-
dc.subject.keywordPlusRADICALS-
dc.subject.keywordPlusKINETICS-
Appears in Collection
MS-Journal Papers(저널논문)
Files in This Item
There are no files associated with this item.
This item is cited by other documents in WoS
⊙ Detail Information in WoSⓡ Click to see webofscience_button
⊙ Cited 3 items in WoS Click to see citing articles in records_button

qr_code

  • mendeley

    citeulike


rss_1.0 rss_2.0 atom_1.0