Journal
ACS CATALYSIS
Volume 7, Issue 11, Pages 7726-7731Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b02647
Keywords
O-2 reduction; electrocatalysis; metal organic framework; porous catalysts; 2D materials
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Funding
- Army Research Office [W911NF-17-1-0174]
- National Science Foundation [1122374]
- DOE
- NIH
- Office of Science, OBES, Division of Chemical Sciences, Geosciences, and Biosciences (CSGB) of the DOE [DE-AC02-05CH11231]
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Establishing catalytic structure function relationships introduces the ability to optimize the catalyst structure for enhanced activity, selectivity, and durability against reaction conditions and prolonged catalysis. Here we present experimental and computational data elucidating the mechanism for the O-2 reduction reaction with a conductive nickel-based metal organic framework (MOF). Elucidation of the O-2 reduction electrokinetics, understanding the role of the extended MOF structure in providing catalytic activity, observation of how the redox activity and pKa of the organic ligand influences catalysis, and identification of the catalyst active site yield a detailed O-2 reduction mechanism where the ligand, rather than the metal, plays a central role. More generally, familiarization with how the structural and electronic properties of the MOF influence reactivity may provide deeper insight into the mechanisms by which less structurally defined nonplatinum group metal electrocatalysts reduce O-2.
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