Exploring highly efficient and ideal stability electrocatalysts for urea oxidation reaction (UOR) is highly desired to achieve hydrogen production by an economic way. Herein, a novel flexible, self-supported NiF₃-Ni₂P heterostructure in-situ grown on carbon cloth (NiF₃/Ni₂P@CC) is controllable synthesized by hydrothermal and subsequent successive fluorination-phosphorization method. The as-obtained optimized NiF₃/Ni₂P@CC-2 is featured by large amounts of high valent Ni³⁺ active sites, reconfigured local charge density, superior hydrophilic surface and mesoporous property. Thanks to these merits, the heterojunction electrode demonstrates advanced UOR performance compared to pure NiF₃@CC and Ni₂P@CC, merely needs a potential of 1.36 V vs. RHE to deliver a current density of 10 mA cm⁻² and keeps the catalytic activity after 5,000 cyclic voltammetry tests. Significantly, NiF₃/Ni₂P@CC-2 hybrid can be utilized as bi-functional catalysts for UOR and water reduction (HER). A symmetrical urea electrolyzer constructed by NiF₃/Ni₂P@CC-2 as anode and cathode offers 50 mA cm⁻² at a potential of 1.83 V, and can work continuously for more than 10 h. This work provides an advanced UOR electrocatalyst and gives great promising for designing heterojunction catalysts for H₂ generation in a more economic way.

探索用于尿素氧化反应（UOR）的高效且理想的稳定性电催化剂是通过经济的方式实现制氢的迫切需要。在此，通过水热和随后的连续氟化-磷化方法可控合成了一种在碳布上原位生长的新型柔性、自支撑 NiF ₃ -Ni ₂ P 异质结构（NiF ₃ /Ni ₂ P@CC）。获得的优化NiF ₃ /Ni ₂ P@CC-2 具有大量高价Ni ³⁺活性位点、重新配置的局部电荷密度、优异的亲水表面和介孔性能。由于这些优点，与纯 NiF ₃ @CC 和 Ni ₂ P@CC相比，异质结电极表现出先进的 UOR 性能，仅需要 1.36 V vs. RHE的电位即可提供 10 mA cm ^-2的电流密度并保持5,000 次循环伏安测试后的催化活性。值得注意的是，NiF ₃ /Ni ₂ P@CC-2 杂化物可用作 UOR 和水还原 (HER) 的双功能催化剂。由 NiF ₃ /Ni ₂ P@CC-2 作为阳极和阴极构建的对称尿素电解槽提供 50 mA cm ^-2电位为1.83 V，可连续工作10小时以上。这项工作提供了一种先进的 UOR 电催化剂，并为以更经济的方式设计用于 H ₂生成的异质结催化剂提供了广阔的前景。