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

Converting CO₂ and H₂ 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 CO₂ reduction is achieved by an element-doped ultrathin metallic photocatalyst-Ni-doped CoS₂ nanosheets (Ni-CoS₂ ). The evolution rate of CH₄ over Ni-CoS₂ is up to 101.8 μmol g⁻¹ h⁻¹ . The metallic and ultrathin nature endow Ni-CoS₂ 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 CH₄ -TPD reveal that the doped Ni atoms in CoS₂ could effectively depress the formation energy of the *COOH, *CHO and desorption energy of CH₄ . 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 CO₂ reduction.