Designing affordable and efficient bifunctional electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has remained a long‐lasting target for the progressing hydrogen economy. Utilization of metal/semiconductor interface effect has been lately established as a viable implementation to realize the favorable electrocatalytic performance due to the built‐in electric field. Herein, a typical Mott–Schottky electrocatalyst by immobilizing Ni/CeO2 hetero‐nanoparticles onto N‐doped carbon nanofibers (abbreviated as Ni/CeO2@N‐CNFs hereafter) has been developed via a feasible electrospinning‐carbonization tactic. Experimental findings and theoretic calculations substantiate that the elaborated constructed Ni/CeO2 heterojunction effectively triggers the self‐driven charge transfer on heterointerfaces, leading to the promoted charge transfer rate, the optimized chemisorption energies for reaction intermediates and ultimately the expedited reaction kinetics. Therefore, the well‐designed Ni/CeO2@N‐CNFs deliver superior HER and OER catalytic activities with overpotentials of 100 and 230 mV at 10 mA cm‐2, respectively, in alkaline solution. Furthermore, the Ni/CeO2@N‐CNFs‐equipped electrolyzer also exhibits a low cell voltage of 1.56 V to attain 10 mA cm‐2 and impressive long‐term durability over 55 h. The innovative manipulation of electronic modulation via Mott–Schottky establishment may inspire the future development of economical electrocatalysts for diverse sustainable energy systems.
Exploring cost‐effective and high‐performance bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of paramount importance for the advancement of H2 production technology, yet remains a huge challenge. Herein, a simple electrospinning–pyrolysis strategy is developed to directly immobilize uniform Ni3Co nanoparticles into a hierarchical branched architecture constructed by in situ formed N‐doped carbon‐nanotube‐grafted carbon nanofibers. The elaborate construction of such hybrid hierarchical architecture can effectively modulate the electronic structure of the active sites, enlarge the exposure of active sites, and facilitate the electron transfer and mass diffusion, favoring both the HER and OER. As a result, the optimized catalyst requires relatively low overpotentials of 114 and 243 mV for HER and OER, respectively, to deliver a current density of 10 mA cm−2 in 0.1 m KOH electrolyte. When employed as a bifunctional catalyst for overall water splitting, the resultant catalyst shows a low cell voltage of 1.57 V to achieve a current density of 10 mA cm−2, along with an impressive stability without noticeable attenuation even after 27 h. This work presents a successful demonstration in optimizing the electrocatalytic performance of Ni‐based bifunctional electrocatalysts by simultaneously considering modulation of electronic structure, hybridization with carbon substrate, and nanostructuring through a facile synthetic strategy, which provides a new avenue to the design of a rich variety of robust transition‐metal‐based electrocatalysts for large‐scale water electrolysis.
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