Dual Redox Active Sites N‐C@Ni2P/NiSe2 Heterostructure Supercapacitor Integrated with Triboelectric Nanogenerator toward Efficient Energy Harvesting and Storage

Abstract Exploring efficient energy systems with integrated energy harvesting and storage toward sustainable power sources is an extremely promising solution for alleviating the energy crisis but nevertheless remains an arduous challenge. Here, a high‐efficient self‐charging power system (SCPS) by integrating solid‐state asymmetric supercapacitors device (SASD) and rotational triboelectric nanogenerator (RTENG) to achieve efficient energy harvesting and storage is reported. Dual redox active sites Ni 2 P/NiSe 2 heterostructure is homogeneously inlaid on N‐C (N‐C@Ni 2 P/NiSe 2 ) via an in situ phosphoselenization, which achieves the maximum exposure of active sites and prevents the aggregation of nanoparticles. The ingeniously designed N‐C@Ni 2 P/NiSe 2 heterostructure features high activity dual redox sites, well‐defined heterointerface, and stable superhighway conductive support, which facilitates high electrochemical reaction efficiency, accelerated reaction kinetics, and enhanced electrochemical stability, thus achieving high capacitance and excellent stability. Meanwhile, the SASD delivers high energy density and long lifespan. Furthermore, the RTENG exhibits high output performance, enabling efficient energy harvesting. The SCPS can reach a voltage of 3.8 V within 40 s, and continuously power electronics. It is believed that the proposed survey based on the design and integration of dual redox active sites heterostructure will offer a new prospect for next‐generation sustainable power sources.