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A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem,Inst Energy Sci & Technol, Dalian 116024, Peoples R China..
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem,Inst Energy Sci & Technol, Dalian 116024, Peoples R China..ORCID iD: 0000-0003-3455-0855
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem,Inst Energy Sci & Technol, Dalian 116024, Peoples R China..
Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem,Inst Energy Sci & Technol, Dalian 116024, Peoples R China..
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2019 (English)In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 10, article id 5074Article in journal (Refereed) Published
Abstract [en]

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 (eta) 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.

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NATURE PUBLISHING GROUP , 2019. Vol. 10, article id 5074
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Chemical Sciences
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URN: urn:nbn:se:kth:diva-264324DOI: 10.1038/s41467-019-13052-1ISI: 000494938800001PubMedID: 31699987Scopus ID: 2-s2.0-85074684201OAI: oai:DiVA.org:kth-264324DiVA, id: diva2:1374564
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QC 20191202

Available from: 2019-12-02 Created: 2019-12-02 Last updated: 2019-12-19Bibliographically approved

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Sun, Licheng

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