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Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH
Stockholm University, Faculty of Science, Department of Organic Chemistry.ORCID iD: 0000-0003-1256-501x
Stockholm University, Faculty of Science, Department of Organic Chemistry.ORCID iD: 0000-0001-5657-8635
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Number of Authors: 172023 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 25, p. 13331-13340Article in journal (Refereed) Published
Abstract [en]

The instability of molecular electrodes under oxidative/reductive conditions and insufficient understanding of the metal oxide-based systems have slowed down the progress of H2-based fuels. Efficient regeneration of the electrode's performance after prolonged use is another bottleneck of this research. This work represents the first example of a bifunctional and electrochemically regenerable molecular electrode which can be used for the unperturbed production of H2 from water. Pyridyl linkers with flexible arms (–CH2–CH2–) on modified fluorine-doped carbon cloth (FCC) were used to anchor a highly active ruthenium electrocatalyst [RuII(mcbp)(H2O)2] (1) [mcbp2− = 2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine]. The pyridine unit of the linker replaces one of the water molecules of 1, which resulted in RuPFCC (ruthenium electrocatalyst anchored on –CH2–CH2–pyridine modified FCC), a high-performing electrode for oxygen evolution reaction [OER, overpotential of ∼215 mV] as well as hydrogen evolution reaction (HER, overpotential of ∼330 mV) at pH 7. A current density of ∼8 mA cm−2 at 2.06 V (vs. RHE) and ∼−6 mA cm−2 at −0.84 V (vs. RHE) with only 0.04 wt% loading of ruthenium was obtained. OER turnover of >7.4 × 103 at 1.81 V in 48 h and HER turnover of >3.6 × 103 at −0.79 V in 3 h were calculated. The activity of the OER anode after 48 h use could be electrochemically regenerated to ∼98% of its original activity while it serves as a HE cathode (evolving hydrogen) for 8 h. This electrode design can also be used for developing ultra-stable molecular electrodes with exciting electrochemical regeneration features, for other proton-dependent electrochemical processes.

Place, publisher, year, edition, pages
2023. Vol. 11, no 25, p. 13331-13340
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Materials Engineering Materials Chemistry
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URN: urn:nbn:se:su:diva-217365DOI: 10.1039/d3ta00071kISI: 000969281800001Scopus ID: 2-s2.0-85153797028OAI: oai:DiVA.org:su-217365DiVA, id: diva2:1759917
Available from: 2023-05-29 Created: 2023-05-29 Last updated: 2023-10-06Bibliographically approved

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Das, BiswanathStåhle, JonasThersleff, ThomasChen, JianhongÅkermark, Björn

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Das, BiswanathStåhle, JonasThersleff, ThomasChen, JianhongDutta, JoydeepÅkermark, Björn
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