We present a controlled fabrication of selective ultrathin metal–organic framework (MOF) nanosheets as preassembling platforms, yolk–shell structured with a few-layered N-doped carbon (NC) shell-encapsulated Ni_0.85Se core (denoted as Ni_0.85[email protected]) via an oriented phase modulation (OPM) strategy. The ultrathin nature of the MOF nanosheets gave rise to the modification of structure at the electronic level with abundant Se-vacancies and effective electronic coupling via an Ni–N_x coordination at the interface between the Ni_0.85Se core and NC shell. The Ni_0.85[email protected] obtained exhibited low overpotentials for both oxygen evolution reaction (OER; 300 mV) and hydrogen evolution reaction (HER; 157 mV) at 10 mA·cm⁻² under an alkaline condition, outperforming their corresponding bulk MOF-derived counterparts. By exploiting Ni_0.85[email protected] as anode and cathode catalysts, a low cell voltage of 1.61 V was achieved by performing alkaline water electrolysis. Remarkably, it also reached a high activity in natural seawater (pH = 7.98) and simulated seawater (pH = 7.86) electrolytes, even surpassing integrated Pt/C-RuO₂/CC electrodes. Density functional theory (DFT) studies illustrated that abundant Se-vacancies effectively regulated the electronic structure of Ni_0.85[email protected] by accelerating electron transfer from Ni to N atoms at the interface, and thus, enabling the Ni_0.85[email protected] to attain a near-optimal electronic configuration that stimulated ideal adsorption-free energy toward key reaction intermediates.

我们提出了一种选择性的超薄金属有机框架（MOF）纳米片作为预组装平台的受控制造方法，该蛋黄壳由几层N掺杂碳（NC）壳包裹的Ni _0.85 Se核（表示为Ni _0.85 [电子邮件通过定向相位调制（OPM）策略。MOF纳米片的超薄特性通过在Ni _0.85 Se核和NC壳层之间的界面处的Ni –N _x配位，在电子水平上具有丰富的Se空位以及有效的电子偶联，从而改变了结构。镍_0.85在碱性条件下，在10 mA·cm ^-2的条件下，所获得的[受电子邮件保护]的氧释放反应（OER; 300 mV）和氢释放反应（HER; 157 mV）均表现出较低的过电势，胜过其相应的大量MOF衍生的对应物。通过使用Ni _0.85 [电子邮件保护]作为阳极和阴极催化剂，通过进行碱性水电解可实现1.61 V的低电池电压。值得注意的是，它在天然海水（pH = 7.98）和模拟海水（pH = 7.86）电解质中也达到了很高的活性，甚至超过了集成的Pt / C-RuO ₂ / CC电极。密度泛函理论（DFT）研究表明，大量的硒空位有效地调节了Ni _0.85的电子结构通过加速界面处Ni到N原子的电子转移来保护电子，从而使Ni _0.85达到接近最佳的电子构型，从而向关键反应中间体激发理想的无吸附能。