期刊
SMALL
卷 19, 期 30, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202300612
关键词
metal-air batteries; oxygen evolution reaction (OER); oxygen reduction reaction (ORR); single-atom catalysts
Anchoring single metal atom to carbon supports is an effective strategy to enhance catalyst efficiency. Dual-atom catalysts (DACs) have emerged as a promising candidate for atomic catalysts, outperforming single-atom catalysts (SACs). However, understanding the structure and benefits of polynary single-atom catalysts remains a challenge.
Anchoring single metal atom to carbon supports represents an exceptionally effective strategy to maximize the efficiency of catalysts. Recently, dual-atom catalysts (DACs) emerge as an intriguing candidate for atomic catalysts, which perform better than single-atom catalysts (SACs). However, the clarification of the polynary single-atom structures and their beneficial effects remains a daunting challenge. Here, atomically dispersed triple Zn-Co-Fe sites anchored to nitrogen-doped carbon (ZnCoFe-N-C) prepared by one-step pyrolysis of a designed metal-organic framework precursor are reported. The atomically isolated trimetallic configuration in ZnCoFe-N-C is identified by annular dark-field scanning transmission electron microscopy and spectroscopic techniques. Benefiting from the synergistic effect of trimetallic single atoms, nitrogen, and carbon, ZnCoFe-N-C exhibits excellent catalytic performance in bifunctional oxygen reduction/evolution reactions in an alkaline medium, outperforming other SACs and DACs. The ZnCoFe-N-C-based Zn-air battery exhibits a high specific capacity (liquid state: 931.8 Wh kg(Zn)(-1)), power density (liquid state: 137.8 mW cm(-2); all-solid-state: 107.9 mW cm(-2)), and good cycling stability. Furthermore, density-functional theory calculations rationalize the excellent performance by demonstrating that the ZnCoFe-N-C catalyst has upshifted d-band center that enhances the adsorption of the reaction intermediates.
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