Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction
Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction
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DOI：
10.1007/s11426-023-1889-6
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发表时间：
2024-01
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通讯作者：
Tong Liu;Yudan Chen;Airong Xu;Xiaokang Liu;Dong Liu;Sicheng Li;Hui Huang;Li Xu;Shuaiwei Jiang;Q. Luo;Tao Ding;Tao Yao
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作者：
Tong Liu;Yudan Chen;Airong Xu;Xiaokang Liu;Dong Liu;Sicheng Li;Hui Huang;Li Xu;Shuaiwei Jiang;Q. Luo;Tao Ding;Tao Yao
探讨致密单原子催化剂（SACs）的原子相互作用机理对其在氧还原反应（ORR）中的应用具有重要意义。然而，位点距离对催化性能影响的内在机理在很大程度上被忽视了。本文从理论上和实验上论证了Fe-Rhx@NC催化剂在ORR中的位距效应。Bader电荷分析表明，一定原子距离上Fe和Rh原子之间的强相互作用（dFe-Rh）改变了催化剂的电子结构，有利于催化剂吸附强度的优化。在理论计算的启发下，我们通过空间约束策略设计并合成了Fe-Rhx@NC催化剂。表征结果证明Fe-Rh2@NC具有最佳的aldfe - rh，提高了其固有ORR活性，提供0.91 V的半波电位，高于商用Pt/C （0.86 V）。本研究强调了确定异金属原子催化剂中位点距离效应的基本机理的重要性，这有助于设计出具有实际应用价值的高效催化剂体系。
Exploring the atomic interaction mechanisms of dense single-atom catalysts (SACs) is of great significance for their application in oxygen reduction reaction (ORR). However, the intrinsic mechanism of the site-distance effect on the catalytic performance has been largely ignored. Here, we demonstrate the site-distance effect of Fe-Rhx@NC catalysts in ORR theoretically and experimentally. Bader charge analysis reveals that the strong interaction between Fe and Rh atoms at a certain atomic distance (dFe-Rh) alters the catalytic electronic structure, facilitating the optimization of catalyst adsorption strength. Motivated by the theoretical calculations, we designed and synthesized the Fe-Rhx@NC catalysts through a spatial confinement strategy. The characterization results prove that the Fe-Rh2@NC has the optimaldFe-Rh, which improves its intrinsic ORR activity, providing a half wave potential of 0.91 V, higher than that of the commercial Pt/C (0.86 V). This study emphasizes the importance of determining the basic mechanism of the site-distance effect in dissimilar metal atoms catalysts, which is conducive to the design of efficient catalyst systems for practical applications.