Reaction-Type-Dependent Behavior of Redox-Hopping in MOFs─Does Charge Transport Have a Preferred Direction?
Year: 2024
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide Redox hopping is the primary method of electron transport through redox-active metal–organic frameworks (MOFs). While redox hopping adequately supports the electrocatalytic application of MOFs, the fundamental understandings guiding the design of redox hopping MOFs remain nascent. In this study, we probe the rate of electron and hole transport through a singular MOF scaffold to determine whether the properties of the MOF promote the transport of one carrier over the other. A redox center, [Ru II (bpy) 2 (bpy-COOH)] 2+, where bpy = 2,2′-bipyridine and bpy-COOH = 4-carboxy-2,2′-bipyridine, was anchored within NU-1000. The electron hopping coefficients ( D e ) and ion diffusion coefficients ( D i ) were calculated via chronoamperometry and application of the Scholz model. We found that electrons transport more rapidly than holes in the studied MOF. Interestingly, the correlation between D e and self-exchange rate built in previous research predicted reversely. The contradicting result indicates that spacing between the molecular moieties involved in a particular hopping process dominates the response.
Institutions: Virginia Tech, Lehigh University
Language: English
Subfield: Inorganic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Awards: G2346589880, NNCI: Virginia Tech National Center for Earth and Environmental Nanotechnology Infrastructure (NanoEarth), Fundamental Investigations into the Metal-Organic Framework Redox-Hopping Charge Transport, G4980309630, G5343152272, G591019902, G6409265431, G67587925, NNCI: The Virginia Tech National Center for Earth and Environmental Nanotechnology Infrastructure (VT NCE2NI)
OpenAlex ID: W4404580581