Polyethylenimine-Modified Bimetallic Au@Rh Core–Shell Mesoporous Nanospheres Surpass Pt for pH-Universal Hydrogen Evolution Electrocatalysis

How to boost the electrocatalytic performance of non-Pt catalysts for the hydrogen evolution reaction (HER) to substitute for Pt is a significant research topic. Herein, by means of the combination of a one-pot wet-chemical method and the post surface functionalization, we successfully fabricate polyethylenimine(PEI)-modified bimetallic Au@Rh core–shell mesoporous nanospheres (Au@Rh@PEI MNs). Benefiting from the synergetic effect of Au@Rh core-shell mesoporous architectures and interfacial modification by PEI molecules, the resultant Au@Rh@PEI MNs exhibit excellent electrocatalytic activity and stability for the HER in all pH value solutions, which even surpass the benchmark commercial Pt/C catalyst. Our synthetic protocol may offer guidelines for rational design of advanced catalysts for water splitting and other electrocatalytic applications.