Atomically Dispersed Pentacoordinated-Zirconium Catalyst with Axial Oxygen Ligand for Oxygen Reduction Reaction

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Abstract

Single-atom catalysts (SACs), as promising alternatives to Pt-based catalysts, suffer from the limited choice of center metals and low single-atom loading. Here, we report a pentacoordinated Zr-based SAC with nontrivial axial O ligands (denoted O−Zr−N−C) for oxygen reduction reaction (ORR). The O ligand downshifts the d-band center of Zr and confers Zr sites with stable local structure and proper adsorption capability for intermediates. Consequently, the ORR performance of O−Zr−N−C prominently surpasses that of commercial Pt/C, achieving a half-wave potential of 0.91 V vs. reversible hydrogen electrode and outstanding durability (92 % current retention after 130-hour operation). Moreover, the Zr site shows good resistance towards aggregation, enabling the synthesis of Zr-based SAC with high loading (9.1 wt%). With the high-loading catalyst, the zinc-air battery (ZAB) delivers a record-high power density of 324 mW cm−2 among those of SAC-based ZABs.

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Wang, X., An, Y., Liu, L., Fang, L., Liu, Y., Zhang, J., … Feng, X. (2022). Atomically Dispersed Pentacoordinated-Zirconium Catalyst with Axial Oxygen Ligand for Oxygen Reduction Reaction. Angewandte Chemie - International Edition, 61(36). https://doi.org/10.1002/anie.202209746

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