A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering

Wenlong Li, Fusheng Li (), Hao Yang, Xiujuan Wu, Peili Zhang, Yu Shan and Licheng Sun ()
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Wenlong Li: Dalian University of Technology
Fusheng Li: Dalian University of Technology
Hao Yang: Dalian University of Technology
Xiujuan Wu: Dalian University of Technology
Peili Zhang: Dalian University of Technology
Yu Shan: Dalian University of Technology
Licheng Sun: Dalian University of Technology

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract 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.

Date: 2019
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DOI: 10.1038/s41467-019-13052-1

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