Abstract
Exploration of high-performance and cost-effective catalysts for hydrogen production from chemical hydrogen-storage materials is vital but still a challenge. Herein we report the synthesis of a ZIF-67 derived Co3O4 nanoparticles in a carbon-based nanoframeworks and discover that doping phosphorus into Co3O4 has a unique electronic structure modulation effect, resulting in a nearly 29-fold enhancement of the catalytic activity for ammonia borane hydrolytic dehydrogenation. Furthermore, combining the P doping with Cu doping, a strong synergistic effect is realized to boost the catalytic H2 generation with an astonishing nearly 51-fold improvement (turnover frequency, TOF = 35.6 min−1). Based on the experimental and theoretical results, the enhanced performance is attributed to the optimization of the electronic configuration and the downshift of d-band center over Co3O4 after P/Cu doping, thereby facilitating H2O dissociation and hydrogen desorption. This work will be applicable to designing other metal based nanocatalysts toward more efficient energy conversion reactions.
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