Designing highly efficient oxygen evolution reaction (OER) electrocatalysts is very important for various electrochemical devices. In this work, for the first time, we have successfully generated coordinatively unsaturated metal sites (CUMSs) in phytic acid–Co²⁺ (Phy–Co²⁺) based metal–organic complexes by engineering the coordination geometry with room-temperature plasma technology. The CUMSs can serve as active centers to catalyze the OER. The electron spin resonance and X-ray absorption spectra provide direct evidence that the coordination geometry is obviously modified with many CUMSs by the plasma treatment. The plasma treated Phy–Co²⁺ (P-Phy–Co²⁺) only requires an overpotential of 306 mV to reach 10 mA cm⁻² on glassy carbon electrodes. When we expand this strategy to a CoFe bimetallic system, it only needs an overpotential of 265 mV to achieve 10 mA cm⁻² with a small Tafel slope of 36.51 mV dec⁻¹. P-Phy–Co²⁺ is superior to the state-of-the-art. Our findings not only provide alternative excellent OER electrocatalysts, but also introduce a promising principle to design advanced electrocatalysts by creating more CUMSs.

中文翻译：

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设计金属-有机络合物电催化剂的配位几何结构，以高度增强氧的释放反应†

设计高效的氧气析出反应（OER）电催化剂对于各种电化学设备非常重要。在这项工作中，我们首次通过使用室温等离子体技术设计配位几何，成功地在基于植酸-Co ²⁺（Phy-Co ²⁺）的金属-有机络合物中成功生成了配位不饱和金属位点（CUMS）。CUMS可以充当催化OER的活跃中心。电子自旋共振和X射线吸收光谱提供了直接的证据，表明通过等离子体处理，许多CUMS明显改变了配位几何形状。经等离子体处理的Phy–Co ²⁺（P-Phy–Co ²⁺）仅需306 mV的超电势即可达到10 mA cm ^-2在玻璃碳电极上。当我们将此策略扩展到CoFe双金属系统时，它仅需要265 mV的超电势即可达到10 mA cm ^-2，而塔菲尔斜率仅为36.51 mV dec ^-1。P-Phy–Co ²⁺优于最新技术。我们的发现不仅提供了替代的优异OER电催化剂，而且通过创建更多CUMS引入了设计先进电催化剂的有希望的原理。