P‐NiFe2O4/N‐doped carbon nanotubes/NiFe multi‐phase heterojunctions for overall water splitting and urea electrolysis

The design and construction of highly efficient electrocatalysts for overall water splitting and urea electrolysis are significantly important for promoting energy conversion and realizing green hydrogen production. In this work, we constructed a multi‐phase heterojunction through a simple hydrothermal and phosphorization process. The P‐doped NiFe2O4 (P‐NiFe2O4) nanoparticles were uniformly anchored on the bamboo‐like N‐doped carbon nanotubes (NCNTs) grown via a NiFe‐alloy autocatalysis. The electronic structure and coordination environment of active species were optimized by the synergistic action of P doping, well‐dispersed ultrafine NiFe2O4, and NCNTs matrix with good conductivity, enhancing their quantity and activity for electrocatalysis. Consequently, the P‐NiFe2O4/NCNTs/NiFe exhibits excellent HER and OER activities with an overpotential of 111 and 266 mV at 10 mA cm‐2 in 1 M KOH, respectively. The symmetrical overall water‐splitting cell using P‐NiFe2O4/NCNTs/NiFe as both anode and cathode delivers 10 mA cm‐2 at a voltage of 1.604 V in 1 M KOH. Notably, the two‐electrode cell requires a low voltage of 1.467 V to achieve a current density of 10 mA cm‐2 in 1 M KOH solution with 0.6 M urea. This designed catalysts display outstanding reaction kinetics and catalytic stability. This work provides useful guidance for applying transition metal‐based catalysts for hydrogen production.