AI Article Synopsis
- Dual-atom catalysts (DACs), specifically dual-atom Fe catalysts (Fe/NC), have shown exceptional catalytic reactivity, but precise fabrication has been challenging.
- A new synthesis method using in situ generated FeCl(g) dimers allows for better control over the Fe-Fe distance in the catalysts, leading to improved performance.
- Research findings indicate that the optimal Fe-Fe distance enhances oxygen adsorption and subsequent reactions, significantly outperforming traditional catalysts like Pt/C.
Article Abstract
Dual-atom catalysts (DACs) have garnered significant interest due to their remarkable catalytic reactivity. However, achieving atomically precise control in the fabrication of DACs remains a major challenge. Herein, we developed a straightforward and direct sublimation transformation synthesis strategy for dual-atom Fe catalysts (Fe/NC) by utilizing in situ generated FeCl(g) dimers from FeCl(s). The structure of Fe/NC was investigated by aberration-corrected transmission electron microscopy and X-ray absorption fine structure (XAFS) spectroscopy. As-obtained Fe/NC, with a Fe-Fe distance of 0.3 nm inherited from FeCl, displayed superior oxygen reduction performance with a half-wave potential of 0.90 V (vs. RHE), surpassing commercial Pt/C catalysts, Fe single-atom catalyst (Fe/NC), and its counterpart with a common and shorter Fe-Fe distance of ~0.25 nm (Fe/NC-S). Density functional theory (DFT) calculations and microkinetic analysis revealed the extended Fe-Fe distance in Fe/NC is crucial for the O adsorption on catalytic sites and facilitating the subsequent protonation process, thereby boosting catalytic performance. This work not only introduces a new approach for fabricating atomically precise DACs, but also offers a deeper understanding of the intermetallic distance effect on dual-site catalysis.
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