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

Wang, Xia; An, Yun; Liu, Lifeng; Fang, Lingzhe; Liu, Yannan; Zhang, Jiaxu; Qi, Haoyuan; Heine, Thomas; Li, Tao; Kuc, Agnieszka; Yu, Minghao; Feng, Xinliang

doi:10.1002/anie.202209746

Title: Atomically Dispersed Pentacoordinated‐Zirconium Catalyst with Axial Oxygen Ligand for Oxygen Reduction Reaction

Journal Article · 28 July 2022 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202209746 · OSTI ID:2470172

Wang, Xia ^[1]; An, Yun ^[2]; Liu, Lifeng ^[3]; Fang, Lingzhe ^[4]; Liu, Yannan ^[5]; Zhang, Jiaxu ^[5]; Qi, Haoyuan ^[6]; Heine, Thomas ^[2]; Li, Tao ^[7];

^[8];

^[5];

^[9]

Technische Universität Dresden (Germany); Max Planck Institute for Chemical Physics of Solids, Dresden (Germany)
Technische Universität Dresden (Germany); Helmholtz-Zentrum Dresden-Rossendorf, Leipzig (Germany)
International Iberian Nanotechnology Laboratory (INL), Braga (Portugal)
Northern Illinois Univ., DeKalb, IL (United States)
Technische Universität Dresden (Germany)
University of Ulm (Germany)
Northern Illinois Univ., DeKalb, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Helmholtz-Zentrum Dresden-Rossendorf, Leipzig (Germany)
Technische Universität Dresden (Germany); Max Planck Institute of Microstructure Physics, Halle (Germany)

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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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: German Research Foundation (DFG); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2470172

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 36 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
high single-atom loading
oxygen reduction reaction
pentacoordinated configuration
single-atom catalysts
zinc-air battery

Title: Atomically Dispersed Pentacoordinated‐Zirconium Catalyst with Axial Oxygen Ligand for Oxygen Reduction Reaction

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References (43)

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