Abstract
CO2 reduction (CO2RR) and hydrogen evolution reactions (HER) are widely used in advanced energy conversion systems, which are urgently required low-cost and high efficient electrocatalysts to overcome the sluggish reaction kinetic and ultralow selectivity. Here, the single-, double-, and triple-atomic Cu embedded graphdiyne (Cu1-3@GDY) complexes have been systematically modeled by first-principles computations to evaluate the corresponding electric structures and catalytic performance. The results revealed that these Cu1-3@GDY monolayers possess high thermal stability by forming the firm Cu–C bonds. The Cu1-3@GDY complexes exhibit good electrical conductivity, which could promote the charge transfer in the electroreduction process. The electronic and magnetic interactions between key species (∗H, ∗COOH, and ∗OCHO) and Cu1-3@GDY complexes are responsible for the different catalytic performance of HER and CO2RR on different Cu1-3@GDY sheets. The Cu2@GDY complex could efficiently convert CO2 to CH4 with a rather low limiting potential of −0.42 V due to the spin magnetism of catalysts. The Cu1@GDY and Cu3@GDY exhibit excellent HER catalytic performance, and their limiting potentials are −0.18 and −0.02 V, respectively. Our findings not only provide a valuable avenue for the design of atomic metal catalysts toward various catalytic reactions but also highlight an important role of spin magnetism in electrocatalysts.
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