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Creators/Authors contains: "Deria, Pravas"

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  1. Free, publicly-accessible full text available August 16, 2024
  2. Free, publicly-accessible full text available June 14, 2024
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  4. Abstract

    Traditional MOF e‐CRR, constructed from catalytic linkers, manifest a kinetic bottleneck during their multi‐electron activation. Decoupling catalysis and charge transport can address such issues. Here, we build two MOF/e‐CRR systems, CoPc@NU‐1000 and TPP(Co)@NU‐1000, by installing cobalt metalated phthalocyanine and tetraphenylporphyrin electrocatalysts within the redox active NU‐1000 MOF. For CoPc@NU‐1000, the e‐CRR responsive CoI/0potential is close to that of NU‐1000 reduction compared to the TPP(Co)@NU‐1000. Efficient charge delivery, defined by a higher diffusion (Dhop=4.1×10−12 cm2 s−1) and low charge‐transport resistance (=59.5 Ω) in CoPC@NU‐1000 led FECO=80 %. In contrast, TPP(Co)@NU‐1000 fared a poor FECO=24 % (Dhop=1.4×10−12 cm2 s−1and=91.4 Ω). For such a decoupling strategy, careful choice of the host framework is critical in pairing up with the underlying electrochemical properties of the catalysts to facilitate the charge delivery for its activation.

     
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  5. Abstract

    Traditional MOF e‐CRR, constructed from catalytic linkers, manifest a kinetic bottleneck during their multi‐electron activation. Decoupling catalysis and charge transport can address such issues. Here, we build two MOF/e‐CRR systems, CoPc@NU‐1000 and TPP(Co)@NU‐1000, by installing cobalt metalated phthalocyanine and tetraphenylporphyrin electrocatalysts within the redox active NU‐1000 MOF. For CoPc@NU‐1000, the e‐CRR responsive CoI/0potential is close to that of NU‐1000 reduction compared to the TPP(Co)@NU‐1000. Efficient charge delivery, defined by a higher diffusion (Dhop=4.1×10−12 cm2 s−1) and low charge‐transport resistance (=59.5 Ω) in CoPC@NU‐1000 led FECO=80 %. In contrast, TPP(Co)@NU‐1000 fared a poor FECO=24 % (Dhop=1.4×10−12 cm2 s−1and=91.4 Ω). For such a decoupling strategy, careful choice of the host framework is critical in pairing up with the underlying electrochemical properties of the catalysts to facilitate the charge delivery for its activation.

     
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  6. Abstract

    Metalorganic frameworks (MOFs) are widely studied molecular assemblies that have demonstrated promise for a range of potential applications. Given the unique and well-established photophysical and electrochemical properties of porphyrins, porphyrin-based MOFs are emerging as promising candidates for energy harvesting and conversion applications. Here we discuss the physical properties of porphyrin-based MOFs, highlighting the evolution of various optical and electronic features as a function of their modular framework structures and compositional variations.

     
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