Atomic Dispersed Co on NC@Cu Core-Shells for Solar Seawater Splitting.

Abstract

With freshwater resources becoming increasingly scarce, the photocatalytic seawater splitting for hydrogen production has garnered widespread attention. In this study, a novel photocatalyst consisting of a Cu core coated is introduced with N-doped C and decorated with single Co atoms (Co-NC@Cu) for solar to hydrogen production from seawater. This catalyst, without using noble metals or sacrificial agents, demonstrates superior hydrogen production effficiency of 9080 µmolg-1h-1, i.e., 4.78% solar-to-hydrogen conversion efficiency, and exceptional long-term stability, operating over 340h continuously. The superior performance is attributed to several key factors. First, the focus-light induced photothermal effect enhances redox reaction capabilities, while the salt-ions enabled charge polarization around catalyst surfaces extends charge carrier lifetime. Furthermore, the Co─NC@Cu exhibits excellent broad light absorption, promoting photoexcited charge production. Theoretical calculations reveal that Co─NC acts as the active site, showing low energy barriers for reduction reactions. Additionally, the formation of a strong surface electric field from the localized surface plasmon resonance (LSPR) of Cu nanoparticles further reduces energy barriers for redox reactions, improving seawater splitting activity. This work provides valuable insights into intergrating the reaction environment, broad solar absorption, LSPR, and active single atoms into a core-shell photocatalyst design for efficient and robust solar-driven seawater splitting.