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dc.contributor.authorEdwardes Moore, Esther
dc.contributor.authorCobb, Samuel
dc.contributor.authorCoito, Ana Margarida
dc.contributor.authorOliveira, Ana Rita
dc.contributor.authorPereira, Ines
dc.contributor.authorReisner, Erwin
dc.date.accessioned2022-02-22T02:04:24Z
dc.date.available2022-02-22T02:04:24Z
dc.date.issued2022-01-25
dc.identifier.issn0027-8424
dc.identifier.otherPMC8795565
dc.identifier.other35058361
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/334309
dc.description.abstractThis work applies electrochemical and computational techniques to explore the local environment of fuel-producing oxidoreductases within porous electrode architectures. This improved understanding of the local environment enabled simple manipulation of the electrolyte solution, by adjusting the bulk pH and buffer pKa, to achieve an optimum local pH for maximal activity of the immobilised enzyme. When applied to macroporous inverse opal electrodes, the benefits of higher loading and increased mass transport were employed and, consequently, the electrolyte adjusted to reach −8.0 mA cm−2 for the H2 evolution reaction (HER) and −3.6 mA cm−2 for the CO2 reduction reaction (CO2RR), demonstrating an 18-fold improvement on previously reported enzymatic CO2RR systems.
dc.languageeng
dc.publisherNational Academy of Sciences
dc.rightsAttribution-NonCommercial-NoDerivatives 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.sourcenlmid: 7505876
dc.sourceessn: 1091-6490
dc.subjectEnzymes
dc.subjectBioelectrochemistry
dc.subjectCo2 Reduction
dc.subjectHydrogen Evolution
dc.subjectLocal Ph
dc.titleUnderstanding the Local Chemical Environment of Bioelectrocatalysis
dc.typeArticle
dc.date.updated2022-02-22T02:04:23Z
prism.issueIdentifier4
prism.publicationNameProceedings of the National Academy of Sciences of USA
prism.volume119
dc.identifier.doi10.17863/CAM.81722
dcterms.dateAccepted2021-11-18
rioxxterms.versionofrecord10.1073/pnas.2114097119
rioxxterms.versionVoR
rioxxterms.licenseref.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.contributor.orcidCobb, Samuel [0000-0001-5015-8090]
dc.contributor.orcidReisner, Erwin [0000-0002-7781-1616]
dc.identifier.eissn1091-6490
pubs.funder-project-idEuropean Research Council (682833)
pubs.funder-project-idLeverhulme Trust (via Imperial College London) (P80336)
cam.issuedOnline2022-01-20


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Attribution-NonCommercial-NoDerivatives 4.0 International
Except where otherwise noted, this item's licence is described as Attribution-NonCommercial-NoDerivatives 4.0 International