Encapsulating Co₂ P@C Core-Shell Nanoparticles in a Porous Carbon Sandwich as Dual-Doped Electrocatalyst for Hydrogen...

A highly efficient and pH-universal hydrogen evolution reaction (HER) electrocatalyst with a sandwich-architecture constructed using zero-dimensional N- and P-dual-doped core-shell Co₂ P@C nanoparticles embedded into a 3 D porous carbon sandwich (Co₂ P@N,P-C/CG) was synthesized through a facile two-step hydrothermal carbonization and pyrolysis method. The interfacial electron transfer rate and the number of active sites increased owing to the synergistic effect between the N,P-dual-doped Co₂ P@C core-shell and sandwich-nanostructured substrates. The presence of a high surface area and large pore sizes improved the mass-transfer dynamics. This nanohybrid showed remarkable electrocatalytic activity toward the HER in a wide pH range with good stability. The computational study and experiments revealed that the carbon atoms close to the N and P dopants on the shell of Co₂ P@N,P-C were effective active sites for HER catalysis and that both Co₂ P and the N,P dopants gave rise to an optimized binding free energy of H on the active sites.