Hydrogen economy by water splitting is the indispensable cornerstone for sustainable energy yet it is impeded by sluggish anodic water oxidation. Hence, the rational design of highly efficient electrocatalysts for oxygen evolution is the key to unlocking its wider use. Herein, cobalt–iron selenide nanoframes are reported for the efficient water oxidation, which need only 270 mV overpotential to give a 10 mA cm⁻² current density and outperforms most cobalt-based catalysts, and even the benchmarked commercial ruthenium oxides (RuO₂). More profoundly, iron doping regulates the local spin state of cobalt species, which further accelerates charge transfer and formation of oxygenated intermediates, and consequently contributes to the enhanced oxygen evolution. This work demonstrates a highly efficient oxygen evolution electrocatalyst and may pioneer a promising approach which involves tuning the local electronic structure to achieve the improved electrocatalysis activities in energy conversion technologies.

中文翻译：

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钴-硒化铁纳米框架的局部自旋态调谐可促进氧的释放

水分解产生的氢经济是可持续能源必不可少的基石，但阳极水氧化反应迟钝阻碍了它的发展。因此，合理设计用于析氧的高效电催化剂是释放其广泛用途的关键。在此，据报道，钴铁硒化物纳米框架可实现有效的水氧化，仅需270 mV的超电势即可产生10 mA cm ^-2的电流密度，并且优于大多数钴基催化剂，甚至优于基准的商业化钌氧化物（RuO ₂）。更深入地讲，铁掺杂调节钴物种的局部自旋状态，这进一步加速了电荷转移和含氧中间体的形成，因此有助于增强氧气的释放。这项工作展示了一种高效的析氧电催化剂，并有望开创一种有前途的方法，该方法涉及调整局部电子结构以实现能量转换技术中改进的电催化活性。