Employing hydrazine oxidation reaction (HzOR) to substitute oxygen evolution reaction (OER) has been regarded as a promising alternative to realize energy-saving hydrogen generation during water splitting. Herein, we introduce a combined experimental and theoretical investigation of zeolitic imidazolate framework-67 coupling with CoNiSe-3 (ZIF67@CoNiSe-3) as an efficient electrocatalyst towards both hydrogen evolution reaction (HER) and HzOR. The as-prepared ZIF67@CoNiSe-3 with nanoflower structure and highly porous ultrathin nanosheet arrays can endow advanced electrocatalytic properties for HER and HzOR. For instance, ZIF67@CoNiSe-3 demands a low overpotential of 49 mV to generate 10 mA·cm^-2 with a small Tafel slope of 41.4 mV·dec^-1 for HER, while it can also reach an ultrahigh current density of 400 mA cm^-2 at 0.13 V vs. reversible hydrogen electrode (RHE) with a small Tafel slope of 44.3 mV·dec^-1 for HzOR. When using ZIF67@CoNiSe-3 as both cathode and anode in a two-electrode cell for overall hydrazine splitting (OHzS), it only needs an ultralow cell voltage of 0.45 V to produce 100 mA·cm^-2 with a remarkable long-term stability of 30 h. Impressively, first-principles calculations (DFT) have been employed to investigate the electrocatalytic mechanisms of ZIF67@CoNi-3 for HER and HzOR. This research could provide an efficient strategy for energy-saving H₂ production during water splitting by incorporating a low-cost yet high-performance bifunctional catalyst.

利用肼氧化反应（HzOR）替代析氧反应（OER）被认为是实现水分解过程中节能制氢的一种有前途的替代方法。在此，我们介绍了沸石咪唑酯骨架 67 与 CoNiSe-3 (ZIF67@CoNiSe-3) 偶联作为析氢反应 (HER) 和 HzOR 的有效电催化剂的实验和理论研究。所制备的 ZIF67@CoNiSe-3 具有纳米花结构和高度多孔的超薄纳米片阵列，可以赋予 HER 和 HzOR 先进的电催化性能。例如，ZIF67@CoNiSe-3 需要 49 mV 的低过电势才能产生 10 mA·cm ^-2以及 41.4 mV·dec ^{-1的小 Tafel 斜率}对于 HER，它还可以在 0.13 V 时达到 400 mA cm ^-2的超高电流密度，相对于可逆氢电极 (RHE)，对于 HzOR ，Tafel 斜率为 44.3 mV·dec ^{-1 。}当使用 ZIF67@CoNiSe-3 作为双电极电池中的正极和负极进行全肼分解 (OHzS) 时，仅需要 0.45 V 的超低电池电压即可产生 100 mA·cm ^-2的电流，具有显着的长期性能稳定性30小时。令人印象深刻的是，第一性原理计算 (DFT) 已被用于研究 ZIF67@CoNi-3 对 HER 和 HzOR 的电催化机制。该研究可以通过结合低成本但高性能的双功能催化剂，为水分解过程中的节能 H _{2生产提供有效的策略。}