Developing Proton-Conductive Metal Coordination Polymer as Highly Efficient Electrocatalyst toward Oxygen Reduction
- 16 September 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry Letters
- Vol. 12 (38), 9197-9204
- https://doi.org/10.1021/acs.jpclett.1c02665
Abstract
Developing earth-abundant transition metal (TM)-based electrocatalysts toward oxygen reduction reaction (ORR) is significant in overcoming the high cost of fuel cells. Herein, using an as-synthesized proton-conductive coordination polymer (termed TM-DHBQ) as a template, we investigate the ORR performance of a series of such TM-DHBQs via screening 3d, 4d, and 5d TMs. We find that most 3d TM-DHBQs exhibit distinguished durability under ORR turnover conditions. The formation energies of these TM-DHBQs and adsorption free energies of ORR intermediates show a good correlation with the number of outer electrons of TM ions in TM-DHBQs, enabling the formation energy as a robust ORR activity descriptor. The Sabatier-type volcano plot and microkinetic modeling coidentify Fe- and Co-DHBQs as two promising alternatives to Pt-based ORR electrocatalysts. For those TM-DHBQs showing strong bonding to oxygen species, the ORR intermediate is found to combine with the TM ion serving as the active center.Funding Information
- Science, Technology and Innovation Commission of Shenzhen Municipality (RCYX20200714114523069, ZDSYS20190902092905285)
- National Natural Science Foundation of China (11974160)
- Guangdong Provincial Key Laboratory for Computational Science and Material Design, Southern University of Science and Technology (2019B030301001)
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