▎ 摘 要
Hydrogen evolution catalysts with effectively integrated structures at different length scales are promising to remarkably boost the efficiency of the hydrogen evolution reaction (HER), but their fabrication presents great challenges. A 3-D structure of graphene oxide (GO) conformally coated with 2,2'-biquinoline-4,4'-dicarboxylate (BQ)-Co2+ complexes is synthesized via polyvinylpyrrolidone (PVP)-mediated in situ self-assembly, in which PVP promotes attachment of BQ and Co2+ and prevents the restacking of nanosheets, while formation of amorphous BQ-Co2+ complexes allows their uniform growth. This structure is subsequently converted to 3-D graphene supported CoP NP-embedded N-doped carbon via calcination and low-temperature phosphidation and applied as a catalyst toward the HER. The onset overpotential, overpotenitial at 10 mA cm(-2), Tafel slope, and exchange current density of this catalyst are 6.3 mV, 78.0 mV, 45.7 mV dec(-1), and 0.3126 mA cm(-2) (0.5 M H2SO4), respectively, all of which compare favorably to those of most reported non-noble-metal-based catalysts, and the catalyst displays superior durability with a slight current increase after 23 h of chronoamperometric measurement or little current loss after 2000 CV cycles. This work develops a strategy to fabricate high-performance and low-cost HER catalysts and deepens the understanding of the mechanism of the polymer-mediated in situ self-assembly of amorphous metal-organic complexes.