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Journal Article

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

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Wang,  Xia
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Wang, X., An, Y., Liu, L., Fang, L., Liu, Y., Zhang, J., et al. (2022). Atomically Dispersed Pentacoordinated-Zirconium Catalyst with Axial Oxygen Ligand for Oxygen Reduction Reaction. Angewandte Chemie, International Edition in English, e202209746, pp. 1-8. doi:10.1002/anie.202209746.


Cite as: https://hdl.handle.net/21.11116/0000-000A-E40F-5
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. © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.