Defects engineering of metal-organic framework immobilized Ni-La(OH)3 nanoparticles for enhanced hydrogen production

Abstract

The development of low-cost, efficient, and durable catalysts to boost hydrogen production from hydrous hydrazine (N2H4·H2O) and hydrazine borane (N2H4BH3) is critical, but still a huge challenge. Herein, for the first time, noble-metal-free La(OH)3-doped Ni nanoparticles (NPs) supported on defect-rich metal−organic framework were constructed via a facile, green, and low-cost wet-chemical method. It is first found that the number of defects in MIL-125(Ti) can be easily regulated by a simple but efficient method. As a result, the defect-rich MIL-125-supported Ni-La(OH)3 catalyst shows superior catalytic activity, 100 % H2 selectivity, and robust durability for N2H4·H2O dehydrogenation with NaOH at 343 K, providing a turnover frequency (TOF) value high up to 870 h−1, surpassing all the non-noble metal catalysts reported so far and even outperforming some noble metal-containing catalysts. Interestingly, the catalyst also shows excellent catalytic efficiency for hydrogen production from N2H4BH3 with a TOF value as high as 2381 h−1 at 343 K. The superior catalytic efficiency is mainly due to the existence of abundant defective MIL-125, electron-rich, good dispersed and small Ni NPs, as well as the synergistic effect between metal and support. This work delivers inspiration in defect engineering and provides a promising strategy for rationally designing high-efficiency MOFs-based catalysts for hydrogen generation and other heterogeneous catalysis.