Reticular Electronic Tuning of Porphyrin Active Sites in Covalent Organic Frameworks for Electrocatalytic Carbon Dioxide Reduction
Why is this work in the frame?
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No Canadian affiliation. An affiliation-only frame — the usual design — would never have seen this work. It is one of the works that make the case for inverting the frame.
Machine scores (provisional)
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- Teacher spread
- 0.257 · how far apart the two teachers sit on this one work
- Validation status
score_only:v0-immature-baseline· verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it
Abstract
The electronic character of porphyrin active sites for electrocatalytic reduction of CO 2 to CO in a two-dimensional covalent organic framework (COF) was tuned by modification of the reticular structure. Efficient charge transport along the COF backbone promotes electronic connectivity between remote functional groups and the active sites and enables the modulation of the catalytic properties of the system. A series of oriented thin films of these COFs was found to reduce CO 2 to CO at low overpotential (550 mV) with high selectivity (faradaic efficiency of 87%) and at high current densities (65 mA/mg), a performance well beyond related molecular catalysts in regard to selectivity and efficiency. The catalysts are stable for more than 12 h without any loss in reactivity. X-ray absorption measurements on the cobalt L-edge for the modified COFs enable correlations between the inductive effects of the appended functionality and the electronic character of the reticulated molecular active sites.
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The record
- Venue
- Journal of the American Chemical Society
- Topic
- Covalent Organic Framework Applications
- Field
- Materials Science
- Canadian institutions
- —
- Funders
- Lawrence Berkeley National LaboratoryArmy Research OfficeBasic Energy SciencesOffice of ScienceEidgenössisches NuklearsicherheitsinspektoratCanadian Institute for Advanced ResearchAcademy of Medical SciencesNational Science FoundationRoyal SocietyKavli FoundationU.S. Department of EnergyBritish Academy
- Keywords
- ChemistryOverpotentialPorphyrinFaraday efficiencySelectivityElectrochemical reduction of carbon dioxideCatalysisCovalent bondCobaltReticular connective tissueCovalent organic frameworkElectrocatalystPhotochemistryInorganic chemistryElectrodeOrganic chemistryElectrochemistryCarbon monoxidePhysical chemistry
- Has abstract in OpenAlex
- yes