Cobalt‐Embedded Nitrogen‐Rich Carbon Nanotubes Efficiently Catalyze Hydrogen Evolution Reaction at All pH Values

Abstract Despite being technically possible, splitting water to generate hydrogen is still practically unfeasible due mainly to the lack of sustainable and efficient catalysts for the half reactions involved. Herein we report the synthesis of cobalt‐embedded nitrogen‐rich carbon nanotubes (NRCNTs) that 1) can efficiently electrocatalyze the hydrogen evolution reaction (HER) with activities close to that of Pt and 2) function well under acidic, neutral or basic media alike, allowing them to be coupled with the best available oxygen‐evolving catalysts—which also play crucial roles in the overall water‐splitting reaction. The materials are synthesized by a simple, easily scalable synthetic route involving thermal treatment of Co 2+ ‐embedded graphitic carbon nitride derived from inexpensive starting materials (dicyandiamide and CoCl 2 ). The materials’ efficient catalytic activity is mainly attributed to their nitrogen dopants and concomitant structural defects.