Electronic structure regulation of nitrogen and phosphorus double doping for N, P-Co4S3/NC nanospheres to enhance all-pH hydrogen evolution

•An effective double ligand strategy was proposed to construct catalyst precursors.•The doping of N and P can regulate the electronic structure of Co.•N from dual ligands can enhance the conductivity and stability of the catalyst.•N, P-Co4S3/NC nanospheres showed outstanding HER performance over the full pH range. In this work, N, P-Co4S3/NC nanospheres were successfully synthesized by double ligand strategy, followed by calcination and phosphating. By adjusting the radio of methimazole and 2-methylimidazole, and changing the calcination temperature, we obtained the optimal hydrogen evolution catalyst. The doping of N and P can regulate the electronic structure of Co, and further improve the electrocatalytic hydrogen production performance. Furthermore, N from dual ligands can form nitrogen-doped carbon, thus enhancing the conductivity and stability of the catalyst. The experimental results showed that N, P-Co4S3/NC exhibited good full pH activity in 0.5 M H2SO4, 1.0 M PBS and 1.0 M KOH, and the overpotentials of 163, 185 and 168 mV were required to reach the current density of 10 mA cm−2, respectively. In this study, the dual ligands strategy can propose a new path for the design and synthesis of the catalyst precursor, and N, P codoping can effectively enhance the catalyst performance. [Display omitted]