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

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.

SUBMITTER: Wang X 

PROVIDER: S-EPMC9543759 | biostudies-literature | 2022 Sep

REPOSITORIES: biostudies-literature