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A flexible cofacial Fe porphyrin dimer as an extremely efficient and selective electrocatalyst for the COto CO conversion in non-aqueous and aqueous media

Journal of Materials Chemistry A, ISSN: 2050-7496, Vol: 9, Issue: 34, Page: 18213-18221
2021
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Metrics Details

  • Citations
    12
    • Citation Indexes
      12
  • Captures
    12

Article Description

Efficient and selective electrochemical reduction of COis a promising approach for its conversion to high value-added chemicals and reducing its green-house effect. Unless a suitable catalyst is used, the reduction occurs at a high overpotential (η) and generates versatile products. Here a novel flexible cofacial Fe perfluorinated porphyrin dimer,f-FePD, was designed for the electrocatalytic CO-to-CO conversion in nonaqueous and aqueous solutions. Thef-FePD showed the CO-to-CO conversion starting at onlyη= 0.15 V that is the lowest reported overpotential in a homogeneous CO-saturated DMF/10% HO/1.0 M PhOH solution. Thisηvalue is 0.29 V lower than that (0.44 V) of the corresponding rigid cofacial Fe porphyrin dimer (r-FePD). Thef-FePD exhibited extremely high turnover frequencies (log TOF) of 2.4 and 7.3 satηvalues of 0.26 and 0.46 V, respectively with >94% CO faradaic efficiency (FE). Moreover, the dimer was immobilized on ketjen black carbon (KBC) and grafted on a glassy carbon (GC) surface to achieve efficient and selective CO-to-CO conversion in neutral aqueous CO-saturated NaHCOsolutions (0.5 M, pH = 7.3) with high durability.f-FePD/KBC@GC showed TOF values of 4.5 and 18.1 swith practical current densities of 3.1 and 12.8 mA cmatηvalues of 0.26 and 0.46 V, respectively. These values, to the best of our knowledge, are the highest reported values achieved in aqueous solutions at such low and moderateηvalues. Several post-operando measurements proved the integrity of thef-FePD under the CO-to-CO conversion conditions. The combination of activity, efficiency, durability, and selectivity of thef-FePD particularly in aqueous solutions is promising for clean energy production.

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