Universal incorporation of metals into cobalt spinel oxide (CSO) has emerged as a versatile and promising strategy to enhance catalytic performance. However, the uncontrolled reactivity of early transition metal and metalloid precursors with water has presented a significant challenge in achieving atomic-scale metal incorporation within CSO. This study presents a groundbreaking approach for the atomic-scale integration of diverse dopants, including Hf, Ta, W, Ti, Pd, Ga, and Ge, while elucidating the atomic stabilization sites for these metal cations within CSO. Notably, certain metals, such as Ta, W, and Ge exhibit greater stability at the surface rather than within the core of CSO, resulting in a Co²⁺-enriched surface that serves as a both catalytically active and protective shell. Exploiting these remarkable features, Ta-doped Co₃O₄ demonstrates the lowest overpotential, registering a mere 378 mV at 10 mA cm⁻², while maintaining its catalytic activity for over 140 hours in acidic electrolyte.

中文翻译：

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通过位点特异性单原子结合定制钴尖晶石氧化物以实现高性能电催化

将金属普遍掺入钴尖晶石氧化物（CSO）中已成为增强催化性能的一种通用且有前途的策略。然而，早期过渡金属和准金属前体与水的不受控制的反应性对在 CSO 中实现原子级金属掺入提出了重大挑战。这项研究提出了一种突破性的方法，用于多种掺杂剂（包括 Hf、Ta、W、Ti、Pd、Ga 和 Ge）的原子级集成，同时阐明了 CSO 中这些金属阳离子的原子稳定位点。值得注意的是，某些金属，例如Ta、W和Ge，在CSO的表面而不是在核心内表现出更大的稳定性，从而形成富含Co ²⁺的表面，该表面既充当催化活性又充当保护壳。利用这些显着的特征，Ta掺杂的Co ₃ O _{4表现出最低的过电势，在10 mA cm} ^-2下仅为378 mV ，同时在酸性电解质中保持其催化活性超过140小时。