Creating Competitive Active Sites on CNTs Walls by N‐Doping and Sublayer Co4N Encapsulating for Efficient Hydrogen Evolution Reaction.

An excellent catalyst can be effectively designed by adjusting its electronic structure. In this paper, an efficient hydrogen evolution reaction (HER) catalyst, carbon nanotubes with N doping and sublayer Co4N encapsulating (N−CNTs@Co4N) supported on Ni foam (NF), was designed and prepared through a complementary electronic structure principle. The as‐prepared N−CNTs@Co4N@NF catalyst shows outstanding hydrogen evolution activity in 1.0 M KOH solution. DFT calculation indicated that carbon nanotubes wall of N−CNTs@Co4N@NF catalyst provided more competitive catalytic active sites for hydrogen evolution reaction than N doped CNTs and Co4N singly. The greatly improved catalytic ability was owing to the redistribution of electron density for N−CNTs after Co4N embeds in, leading to a moderate absorption energy of H. This study demonstrated the successful rational design and experimental verification on developing a novel non‐noble metal catalyst. [ABSTRACT FROM AUTHOR]