Copper-Induced Structure Evolution of Catalysts for Boosting Hydrogen Generation

Hydrogen is considered sustainable and clean energy because of its advantages of environmental friendliness and high calorific value. Designing high-efficiency catalysts and understanding the structure–activity relationship of catalysts are paramount issues for hydrogen generation from ammonia borane hydrolysis. Herein, effective catalysts were designed for hydrogen generation by utilization of the dynamic structural evolution during the reaction. The promotional effects of the Cu component were specifically studied to provide insights into the structure–activity relationship. Screening of various metallic additives (Ni, Mo, Fe, Mn, Ce, and Mg) demonstrated their negligible impact on catalytic performance, whereas Cu emerged as an exclusively critical component for enabling hydrogen evolution activity due to its role in promoting reduction. The optimized CoCu_0.4Pt_0.04-O-400 achieved a turnover frequency value of 4326 min^–1 at 298 K and an E_a of 32.48 kJ·mol^–1 and exhibited excellent recyclability. The formed interfacial Pt–Cu–CoO sites in catalysts induced by dynamic structural evolution enhanced the activation of H₂O and NH₃BH₃ molecules, which boosted the catalytic activity. This work showcases a facile and green method for the development of effective and sustainable catalysts and provides insight into the structure–activity relationship of catalysts in ammonia borane hydrolysis.