Nickel-Based Water-Soluble Metallopolymer for the Electrochemical Hydrogen Evolution Reaction in Neutral-pH Water AITranslate

Basic Information:

DOI：https://doi.org/10.1021/acsapm.1c00820

Chinese Library Classification Number:

Citation Information:

Electrochemical production of the energy-dense hydrogen molecule in green solvents such as water, under mild conditions, has been desirable but challenging. A burgeoning family of catalysts that currently serve in such hydrogen evolution reactions (HERs) are artificial metalloenzymes and metallopolymers, which were manifested through the direct syntheses between HER-active metal complexes and protein matrices or water-soluble polymers. The direct synthetic method often poses some limitations on active site variants and synthetic feasibility. Here, we propose the first HER-active metallopolymer catalyst manifested through the bottom-up synthetic strategy and a facile postpolymerization modification. With the advent of this method, the tridentate ligation (N-[2-(aminopropylthio)phenyl]-2-pyridinemethamine (NNS-PrNH2)) and the water-solubilizing (amino-containing poly(ethylene glycol) (PEG-NH2)) pendent units were furnished onto polymer backbone with quantitative precision. The readily synthesized polymers were self-folding in water, and subsequently formed the polymeric nanoassemblies upon nickel-coordination complexation to give a high concentration of active sites in hydrophobic compartments. The stable metallopolymers showed practical usage in the electrochemical HER in a pH 7 aqueous solution, under ambient conditions, resulting in 41 ± 9 μmol of H2 evolved in 1 h with the satisfactory faradaic efficiencies of 58 ± 2%.