The hybridization with conductive nanostructures has attracted intense research interest because of its high efficiency in the exploration of efficient energy-functional materials. In this study, we reported a high efficacy of substrate dimensionality control in optimizing the specific capacitance and phase stability of hybridized nanostructures. Employing defective holey TiN nanostructures as substrates was found to enhance the interfacial interactions with a hybridized layered double hydroxide (LDH). A comparative investigation of two-dimensional TiN-LDH nanohybrids with zero-dimensional/one-dimensional TiN-LDH homologs demonstrated that hybridization with holey two-dimensional TiN nanosheets led to a much greater specific capacitance of 2127 F g⁻¹, which is one of the best performances among LDH-based electrodes ever-reported. In situ Raman analysis during electrochemical cycling clearly demonstrated that holey nanosheet morphology of TiN substrate is quite crucial in promoting the phase transition of hybridized Ni-Fe-LDH to NiOOH/FeOOH with the maximization of cation redox activities. These advantages of atomically thin holey TiN nanosheets could be ascribed to intimate electronic coupling at the bilateral interfaces of the two-dimensional LDH nanosheets, in addition to optimized porosity and improved mass transport.

与导电纳米结构的杂化因其在探索高效能量功能材料方面的高效率而引起了强烈的研究兴趣。在这项研究中，我们报道了衬底尺寸控制在优化杂化纳米结构的比电容和相稳定性方面的高效性。发现采用有缺陷的多孔 TiN 纳米结构作为基底可以增强与杂化层状双氢氧化物(LDH)的界面相互作用。二维 TiN-LDH 纳米杂化物与零维/一维 TiN-LDH 同系物的比较研究表明，与多孔二维 TiN 纳米片的杂化导致比电容大得多，为 2127 F g ⁻¹，这是迄今为止报道的基于 LDH 的电极中性能最好的之一。电化学循环过程中的原位拉曼分析清楚地表明，TiN 基板的多孔纳米片形态对于促进杂化的 Ni-Fe-LDH 向 NiOOH/FeOOH 的相变以及阳离子氧化还原活性的最大化至关重要。原子级薄的多孔 TiN 纳米片的这些优势可归因于二维 LDH 纳米片双边界面处的紧密电子耦合，以及优化的孔隙率和改进的传质。