Exploring electrocatalysts with optimal electronic structure and understanding the relationship between electronic structure and activity are highly required for designing advanced OER catalysts. Recently, introducing nanocarbon materials into LDHs has been demonstrated as an effective way to improve the OER activity; however, deeply understanding the regulating effect of nanocarbon on the electronic structure of LDHs is still a critical challenge. Herein, it is reported that the regulating of the surface electronic structure of nickel-based layered double hydroxides (NiM-LDHs (M = Fe, Co, Mn)) by adsorbing graphene quantum dot (GQDs). The Ni-based LDHs/GQDs delivers enhanced OER activity, and particularly NiFe LDH/GQDs achieves an ultralow overpotential of 189 mV (10 mA cm⁻²) and superior performance in rechargeable Zn–air battery tests. Combining with theoretical calculations and X-ray photoelectron spectroscopy, we ascribe the excellent OER activity of Ni-based LDHs/GQDs to the strong interaction between NiFe LDH and GQDs, which changes the charge distribution around metal ions and triggers the charge accumulation of the active Ni species. The above results demonstrate the significance of controlling the surface electronic structure for designing advanced 3d metal electrocatalysts.

设计先进的OER催化剂非常需要探索具有最佳电子结构的电催化剂，并了解电子结构与活性之间的关系。最近，已证明将纳米碳材料引入LDHs是提高OER活性的有效方法。然而，深入了解纳米碳对LDHs电子结构的调节作用仍然是一个严峻的挑战。此处，据报道，通过吸附石墨烯量子点（GQD）来调节镍基层状双氢氧化物（NiM-LDHs（M ＝ Fe，Co，Mn））的表面电子结构。镍基LDH / GQD提供增强的OER活性，尤其是NiFe LDH / GQD实现189 mV（10 mA cm ^-2）的超低过电势）和可充电锌空气电池测试中的卓越性能。结合理论计算和X射线光电子能谱，我们将镍基LDH / GQD的出色的OER活性归因于NiFe LDH和GQD之间的强相互作用，从而改变了金属离子周围的电荷分布并触发了活性物质的电荷积累镍种。以上结果证明了控制表面电子结构对于设计先进的3d金属电催化剂的重要性。