Modulating the electronic structures of cobalt-organic frameworks for efficient electrocatalytic oxygen evolution

Improved electronic structures of Co-based MOFs by the controllable introduction of Ce lead to excellent OER performance with an ultra-low overpotential of 285 mV at 10 mA·cm−2, a favorable Tafel slope of 56.1 mV·dec−1, and superior stability, outperforming precious IrO2 and most of the reported met...

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Veröffentlicht in:Journal of colloid and interface science 2023-11, Vol.650 (Pt B), p.1949-1957
Hauptverfasser: Hao, Yongchao, Guo, Zhongyuan, Cheng, Huiya, Yao, Chenghao, Cheng, Shuling, Yi, Lizhi, Li, Hao
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Sprache:eng
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Zusammenfassung:Improved electronic structures of Co-based MOFs by the controllable introduction of Ce lead to excellent OER performance with an ultra-low overpotential of 285 mV at 10 mA·cm−2, a favorable Tafel slope of 56.1 mV·dec−1, and superior stability, outperforming precious IrO2 and most of the reported metal-based catalysts. [Display omitted] The oxygen evolution reaction (OER) is a key process in various energy storage/generation technologies. Tuning the electronic structures of catalysts is an effective approach to improve the catalyst’s activity. In this work, we synthesized Ce-doped cobalt-organic frameworks with benzene-1, 4-dicarboxylic acid (BDC) as the ligand as efficient OER electrocatalysts (denoted as Co3Ce1 BDC) with excellent stability and improved catalytic performance. The introduced Ce in Co3Ce1 BDC changes the surface configuration and tunes electronic structures of the active Co site, leading to enhanced interaction between intermediates and catalysts. Besides, the specific surface area, reaction kinetics, charge transfer efficiency, and turnover frequency are also improved in the presence of Ce. As a result, the Co3Ce1 BDC demonstrated excellent performance with a low overpotential of 285 mV at a current of 10 mA·cm−2, a preferable Tafel slope of 56.1 mV·dec−1, and an excellent durability in 1 M KOH, indicating the potential for practical applications in water splitting and other energy storage technologies wherein the OER plays a critical role. Comprehensive theoretical calculations and modeling further identified the key role of Ce in modulating the electronic structure and OER activity of cobalt-organic frameworks. Most importantly, this work provides a new strategy to the development of efficient cobalt-organic framework catalysts in OER-related applications.
ISSN:0021-9797
1095-7103
DOI:10.1016/j.jcis.2023.07.151