Heteroatomic anion doping represents a powerful approach for manipulating the electronic configuration of the active metal locus in electrocatalysts, resulting in enhanced multifunctional electrocatalytic properties in hydrogen/oxygen evolution reactions (HER/OER). Here, fluorine-tailored Ni₂P-F3 nanosheets were synthesized and evaluated as a robust multifunctional electrocatalyst for HER, OER, and UOR. Our comprehensive experimental and theoretical investigations reveal that the anionic F effectively tailored the electronic states of the Ni₂P-F3 nanosheets, resulting in an elevated d-band center and optimizing the sorption capacity of intermediates. In addition to thermodynamically and kinetically favoured redox reactions, F doping facilitates the reconstruction and generation of active γ-NiOOH. Resulting from the optimized electronic configuration and nanosheet architecture, outstanding catalytic activities are demonstrated by Ni₂P-F3 with low overpotentials to reach 100 mA cm⁻² for HER (177 mV) and OER (293 mV), surpassing Ni₂P by 234 and 205 mV, respectively. Notably, 1.618 V is required for full-water-diversion to reach 10 mA cm⁻², while 1.414 V is required with urea oxidation for 100 mA cm⁻².

中文翻译：

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F调节的Ni2P-F3纳米片作为全水分解和尿素氧化的高效电催化剂

杂原子阴离子掺杂是操纵电催化剂中活性金属位点电子构型的有效方法，从而增强析氢/析氧反应（HER/OER）中的多功能电催化性能。在这里，合成了氟定制的 Ni ₂ P-F3 纳米片，并将其作为 HER、OER 和 UOR 的稳健多功能电催化剂进行了评估。我们全面的实验和理论研究表明，阴离子 F 有效地调整了 Ni ₂ P-F3 纳米片的电子态，从而提高了 d 带中心并优化了中间体的吸附能力。除了热力学和动力学上有利的氧化还原反应之外，F 掺杂还促进活性 γ-NiOOH 的重建和生成。由于优化的电子配置和纳米片结构，Ni ₂ P-F3表现出出色的催化活性，其过电势较低，对于 HER (177 mV) 和 OER (293 mV)达到 100 mA cm ^{-2 ，比 Ni} ₂ P 高出 234和205毫伏，分别。值得注意的是，完全分水达到10 mA cm ^-2需要1.618 V，而尿素氧化达到100 mA cm ^-2需要1.414 V。