Enhancing the d/p-Band Center Proximity with Amorphous-Crystalline Interface Coupling for Boosted pH-Robust Water Electrolysis

Rationalizing non-precious pH-robust electrocatalysts is a crucial priority and required for multi-scenario hydrogen production customization. Herein, an amorphous-crystalline CoBOx/NiSe heterostructure is theoretically profiled and constructed for efficient and pH-robust water electrolysis. The crystalline lattice confinement induces a Co-Co bond shortening and a B-site delocalization on amorphous CoBOx, resulting in a decreased d-p band center difference (Delta epsilon(d-p)) toward the balanced intermediates adsorption/desorption. Accordingly, the CoBOx/NiSe heterostructure exhibits efficient and robust hydrogen/oxygen evolution reaction (HER/OER) catalytic activity in different electrolytes. Of particular note, it achieves ultralow overpotentials in both the beyond-Pt HER (14.5 mV) and OER (229.1 mV) at 10 mA cm(-2) under an alkaline electrolyte, and reaches an industrial-level OER current density of 2 A cm(-2). Water electrolysis is stably delivered with a low eta(10) voltage of 1.48 V. The incorporation of such d-p orbitals at the amorphous-crystalline interface puts forward new opportunities in rationally designing advanced non-precious electrocatalysts for water electrolysis.

Automated summary

Researchers have developed a non-precious pH-robust electrocatalyst for efficient and stable water electrolysis. This catalyst exhibits excellent catalytic activity for hydrogen and oxygen evolution reactions in alkaline electrolytes, achieving ultralow overpotentials and high OER current density.