Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 24, Issue 43, Pages 10984-10987Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201802585
Keywords
catalysis; heterogeneous; oxygen reduction; porphyrin; self-assembly
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Funding
- Department of Energy Office of Science [DE-AC02-05CH11231]
- University at Buffalo
- State University of New York Research Foundation
- National Center For Research Resources [S10RR029517]
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We report a suite of coordination-driven self-assembled prisms for heterogeneous electrocatalytic oxygen reduction (ORR) differing in the molecular clips linking two porphyrin faces in a cofacial arrangement. ORR activities and selectivities of monomeric CoTPyP along with cofacial prisms Ox-Co, Oxa-Co, and Benzo-Co were probed using cyclic voltammetry and rotating ring-disk techniques. All species were immobilized as heterogeneous catalysts on glassy carbon electrodes using a Nafion ink method. The selectivities of Ox-Co, Oxa-Co, and Benzo-Co prisms towards H2O as determined by RRDE were 87, 97, and 75%, respectively. The current density of the Oxa-Co plateaus at five times that of Pt/C when normalized per Co/Pt. The high synthetic yield (79%), competitive overpotential (eta approximate to 800 mV) and high selectivity (%H2O approximate to 97%) of the Oxa-Co highlights how self-assembly can be used to address multi-electron multi-proton transformations using polynuclear catalysts.
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