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dc.contributor.authorCobb, Samuel
dc.contributor.authorBadiani, Vivek
dc.contributor.authorDharani, Azim M
dc.contributor.authorWagner, Andreas
dc.contributor.authorZacarias, Sónia
dc.contributor.authorOliveira, Ana Rita
dc.contributor.authorPereira, Inês AC
dc.contributor.authorReisner, Erwin
dc.date.accessioned2022-01-12T00:30:49Z
dc.date.available2022-01-12T00:30:49Z
dc.date.issued2022-04
dc.identifier.issn1755-4330
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/332637
dc.description.abstractThe performance of heterogeneous catalysts for electrocatalytic CO2 reduction suffers from unwanted side reactions and kinetic inefficiencies at the required large overpotential. However, immobilized CO2 reduction enzymes-such as formate dehydrogenase-can operate with high turnover and selectivity at a minimal overpotential and are therefore 'ideal' model catalysts. Here, through the co-immobilization of carbonic anhydrase, we study the effect of CO2 hydration on the local environment and performance of a range of disparate CO2 reduction systems from enzymatic (formate dehydrogenase) to heterogeneous systems. We show that the co-immobilization of carbonic anhydrase increases the kinetics of CO2 hydration at the electrode. This benefits enzymatic CO2 reduction-despite the decrease in CO2 concentration-due to a reduction in local pH change, whereas it is detrimental to heterogeneous catalysis (on Au) because the system is unable to suppress the H2 evolution side reaction. Understanding the role of CO2 hydration kinetics within the local environment on the performance of electrocatalyst systems provides important insights for the development of next-generation synthetic CO2 reduction catalysts.
dc.publisherSpringer Science and Business Media LLC
dc.rightsAll Rights Reserved
dc.rights.urihttp://www.rioxx.net/licenses/all-rights-reserved
dc.titleFast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis.
dc.typeArticle
dc.publisher.departmentDepartment of Chemistry
dc.date.updated2022-01-10T17:07:40Z
prism.publicationNameNat Chem
dc.identifier.doi10.17863/CAM.80082
dcterms.dateAccepted2021-12-15
rioxxterms.versionofrecord10.1038/s41557-021-00880-2
rioxxterms.versionAM
dc.contributor.orcidCobb, Samuel [0000-0001-5015-8090]
dc.contributor.orcidBadiani, Vivek [0000-0002-3867-6714]
dc.contributor.orcidDharani, Azim M [0000-0003-2012-146X]
dc.contributor.orcidReisner, Erwin [0000-0002-7781-1616]
dc.identifier.eissn1755-4349
rioxxterms.typeJournal Article/Review
pubs.funder-project-idEuropean Research Council (682833)
pubs.funder-project-idLeverhulme Trust (via Imperial College London) (P80336)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L016087/1)
cam.issuedOnline2022-02-28
datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.78484
cam.orpheus.successWed Mar 23 10:26:22 GMT 2022 - Embargo updated
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cam.depositDate2022-01-10
pubs.licence-identifierapollo-deposit-licence-2-1
pubs.licence-display-nameApollo Repository Deposit Licence Agreement
rioxxterms.freetoread.startdate2022-08-28


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