Atom-Pd catalysts supported by hollow N-doped carbon nanospheres for ultra-efficient nitrogen reduction reaction

Abstract

Electrochemical N2 reduction reaction (eNRR) presents a promising alternative to the Haber-Bosch process, owing to its mild preparation conditions, absence of costly reagents, and high energy conversion efficiency. However, the process poses significant challenges due to its poor selectivity and low yield. Here, single atom Pd is successfully anchored on N-doped hollow carbon nanospheres via a simple wet impregnation method under relatively mild loading temperature, anhydrous and anaerobic environments. Our experiment demonstrates that SA-Pd/N@C exhibits outstanding catalytic performance in comparison to Pd nanoparticles which is consistent with the results of the DFT calculations, achieving an NH3 yield rate of 132.8 μg·h − 1·mgcat−1 and a corresponding FE of 6 % at -0.2 V versus RHE in HCl electrolyte (pH=1), as well as superior stability with only 5 % decrease after 10 consecutive cycles of electrochemical testing at room temperature, positioning it as one of the most effective catalyst materials reported for eNRR. The exceptional eNRR activity and stability can be attributed to the abundant active sites resulting from the relatively mild loading temperature, as well as electronic effects and structural engineering, which further diminish *H adsorption and efficiently suppress hydrogen evolution reaction. This work will provide a novel approach to enhance the eNRR performance through the effective design of Pd single-atom catalyst