Efficient Infrared‐Light‐Driven CO2 Reduction Over Ultrathin Metallic Ni‐doped CoS2 Nanosheets

Abstract Converting CO 2 and H 2 O into carbon‐based fuel by IR light is a tough task. Herein, compared with other single‐component photocatalysts, the most efficient IR‐light‐driven CO 2 reduction is achieved by an element‐doped ultrathin metallic photocatalyst‐Ni‐doped CoS 2 nanosheets (Ni‐CoS 2 ). The evolution rate of CH 4 over Ni‐CoS 2 is up to 101.8 μmol g −1 h −1 . The metallic and ultrathin nature endow Ni‐CoS 2 with excellent IR light absorption ability. The PL spectra and Arrhenius plots indicate that Ni atoms could facilitate the separation of photogenerated carriers and the decrease of the activation energy. Moreover, in situ FTIR, DFT calculations, and CH 4 ‐TPD reveal that the doped Ni atoms in CoS 2 could effectively depress the formation energy of the *COOH, *CHO and desorption energy of CH 4 . This work manifests that element doping in atomic level is a powerful way to control the reaction intermediates, providing possibilities to realize high‐efficiency IR‐light‐driven CO 2 reduction.