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A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
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A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
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A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
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Journal Article
A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
2019
Overview
First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials (
η
) significantly above thermodynamic requirements. Here, we report an iron/nickel terephthalate coordination polymer on nickel form (
NiFeCP/NF
) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis.
NiFeCP/NF
exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm
−2
in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of
NiFeCP/NF
on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate.
Proton-coupled electron transfer (PCET) process is very important for water oxidation catalysis. Here, the authors introduced uncoordinated carboxylate in the second-coordination-sphere of Ni-Fe coordination polymer catalyst as an internal base to promote the water oxidation kinetics by such PCET process.
