Efficient Solar‐Driven CO2 Methanation and Hydrogen Storage Over Nickel Catalyst Derived from Metal–Organic Frameworks with Rich Oxygen Vacancies.

Solar‐driven photothermal conversion of carbon dioxide (CO2) to methane (CH4) is a promising approach to remedy energy shortage and climate changes, where highly efficient photothermal catalysts for CO2 methanation urgently need to be designed. Herein, nickel‐based catalysts (Ni/ZrO2) derived from metal–organic frameworks (MOFs) are fabricated and studied for photothermal CO2 methanation. The optimized catalyst 50Ni/ZrO2 achieves a stable CH4 production rate of 583.3 mmol g−1 h−1 in a continuous stability test, which is almost tenfold higher than that of 50Ni/C‐ZrO2 synthesized via commercial ZrO2. Physicochemical properties indicate that 50Ni/ZrO2 generates more tetragonal ZrO2 and possesses more oxygen vacancies (OVs) as well as enhanced nickel‐ZrO2 interaction. As a result, 50Ni/ZrO2 exhibits the strong abilities of light absorption and light‐to‐heat conversion, superior adsorption capacities of reactants (H2, CO2), and an intermediate product (CO), which finally boosts CH4 formation. This work provides an efficient strategy to design a photothermocatalyst of CO2 methanation through utilizing MOFs‐derived support. [ABSTRACT FROM AUTHOR]