Boron-Induced Electronic-Structure Reformation of CoP Nanoparticles Drives Enhanced pH-Universal Hydrogen Evolution
Erping Cao1, Zhimin Chen1, Hao Wu1
1Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education of China), School of Chemistry and Materials Science, Heilongjiang University, Harbin, 150080, P. R. China.
Abstract:
Even though transition-metal phosphides (TMPs) have been developed as promising alternatives to Pt catalyst for the hydrogen evolution reaction (HER), further improvement of their performance requires fine regulation of the TMP sites related to their specific electronic structure. Herein, for the first time, boron (B)-modulated electrocatalytic characteristics in CoP anchored on the carbon nanotubes (B-CoP/CNT) with impressive HER activities over a wide pH range are reported. The HER performance surpasses commercial Pt/C in both neutral and alkaline media at large current density (>100 mA cm-2 ). A combined experimental and theoretical study identified that the B dopant could reform the local electronic configuration and atomic arrangement of bonded Co and adjacent P atoms, enhance the electrons' delocalization capacity of Co atoms for high electrical conductivity, and optimize the free energy of H adsorption and H2 desorption on the active sites for better HER kinetics.
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