Loading Nickel Atoms on GDY for Efficient CO2 Fixation and Conversion

Carbon dioxide(CO₂) is an important and valuable C1 resource for the synthesis of numerous of value-added products. However, efficient fixation and conversion of CO₂ into organic carbonates under mild conditions remain great challenges. Herein, graphdiyne(GDY)-based nickel atomic catalysts(Ni⁰/GDYs) were synthesized through a facile in-situ reduction method. Experimental results showed that the obtained Ni⁰/GDY had outstanding catalytic performances for converting CO₂ into cyclic carbonates with a high reaction conversion(99%) and reaction selectivity(ca. 100%) at 80℃ and under 1 atm(1 atm=101325 Pa). Specially, the activation energy (E_a) value for the Ni⁰/GDY is 37.05 kJ/mol, lower than those of reported catalysts. The reaction mechanism was next carefully analyzed by using density functional theory(DFT) calculations. Such an excellent catalytic property could be mainly attributed to the high dispersion of active sites on the Ni⁰/GDY, and the unique incomplete charge transfer properties of GDY-based zero-valent metallic catalysts.