Polydopamine‐Inspired, Dual Heteroatom‐Doped Carbon Nanotubes for Highly Efficient Overall Water Splitting

Overall water splitting involved hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are critical for renewable energy conversion and storage. Heteroatom‐doped carbon materials have been extensively employed as efficient electrocatalysts for independent HER or OER processes, while those as the bifunctional catalysts for simultaneously generating H 2 and O 2 by splitting water have been seldom reported. Inspired by the unparalleled virtues of polydopamine, the authors devise the facile synthesis of nitrogen and sulfur dual‐doped carbon nanotubes with in situ, homogenous and high concentration sulfur doping. The newly developed dual‐doped electrocatalysts display superb bifunctional catalytic activities for both HER and OER in alkaline solutions, outperforming all other reported carbon counterparts. Experimental characterizations confirm that the excellent performance is attributed to the multiple doping together with efficient mass and charge transfer, while theoretical computations reveal the promotion effect of secondary sulfur dopant to enhance the spin density of dual‐doped samples and consequently to form highly electroactive sites for both HER and OER.