A Novel Multinary Intermetallic as an Active Electrocatalyst for Hydrogen Evolution.

Abstract

Electrochemical water splitting offers an attractive approach for hydrogen production. However, the lack of high-performance cost-effective electrocatalyst severely hinders its applications. Here, a multinary high-entropy intermetallic (HEI) that possesses an unusual periodically ordered structure containing multiple non-noble elements is reported, which can serve as a highly efficient electrocatalyst for hydrogen evolution. This HEI exhibits excellent activities in alkalinity with an overpotential of 88.2 mV at a current density of 10 mA cm-2 and a Tafel slope of 40.1 mV dec-1 , which are comparable to those of noble catalysts. Theoretical calculations reveal that the chemical complexity and surprising atomic configurations provide a strong synergistic function to alter the electronic structure. Furthermore, the unique L12 -type ordered structure enables a specific site-isolation effect to further stabilize the H2 O/H* adsorption/desorption, which dramatically optimizes the energy barrier of hydrogen evolution. Such an HEI strategy uncovers a new paradigm to develop novel electrocatalyst with superior reaction activities.