近日，课题组硕士生张华硕论文“N, S coordination in Co single atom catalyst promoting CO2RR towards HCOOH at negative potentials”被Molecular Catalysis（中科院SCI期刊三区期刊，IF=3.9）接收！
Co-based single-atom catalysts (Co-SACs) have attracted widespread attention in electrocatalytic CO2 reduction reaction (CO2RR). The coordination environment around Co active centers plays a crucial role in determining their intrinsic catalytic activity. This work systematically investigates the effect of introducing different numbers of S atoms into the Co-N4 coordination environment (Co-NxS4-x, x = 1––4) on the CO2RR performance at negative potentials. Among all structures, para-sulfur doped structure (p-CoN2S2) performs best with the limiting potentials for HCOOH generation of –0.19, 0, and 0 V at –0.23, –0.54, and –0.84 V, respectively. Compared to CoN4, the substitution of S atoms in p-CoN2S2 results in the emergence of two electron distribution peaks at –0.46 and –0.02 eV, primarily contributed by the Co 2p and 3d orbitals. This significantly reduces the band gap of p-CoN2S2 to 0.36 eV, much lower than that of CoN4 (1.82 eV), thereby enhancing the electrical conductivity. Additionally, p-CoN2S2 exhibits a higher occupation of the Co 3d orbital, which is beneficial for the electron transfer from Co atom to CO2, thus promoting CO2RR. This work highlights p-CoN2S2 as an efficient catalyst for HCOOH production, and demonstrates that the N, S coordination is an effective strategy to modulate the CO2RR performance at negative potentials.
https://doi.org/10.1016/j.mcat.2025.115137
