Functional Group Regulated Ni/Ti3C2Tx (Tx = F, -OH) Holding Bimolecular Activation Tunnel for Enhanced Ammonia Borane Hydrolysis

Developing economical and efficient catalyst for hydrogen generation from ammonia borane (AB) hydrolysis is still a huge challenge. As an alternative strategy, the functional group regulation of metal nanoparticles (NPs)-based catalysts is believed to be capable of improving the catalytic activity. Herein, a series of Ni/Ti3C2Tx-Y (T-x = F, -OH; Y denotes etching time (d)) catalysts are synthesized and show remarkably enhanced catalytic activity on the hydrolysis of AB in contrast to the corresponding without regulating. The optimized Ni/Ti3C2Tx-4 with a turnover frequency (TOF) value of 161.0 min(-1) exhibits the highest catalytic activity among the non-noble monometallic-based catalyst. Experimental results and theory calculations demonstrate that the excellent catalytic activity benefits from the bimolecular activation channels formed by Ni NPs and Ti3C2Tx-Y. H2O and AB molecules are activated simultaneously in the bimolecular activation tunnel. Bimolecular activation reduces the activation energy of AB hydrolysis, and hydrogen generation rate is promoted. This article provides a new approach to design effective catalysts and further center dot supports the bimolecular activation model for the hydrolysis of AB.

Automated summary

This study successfully synthesized a series of catalysts with regulated functional groups for hydrogen generation from ammonia borane hydrolysis, showing significantly enhanced catalytic activity. The optimized catalyst exhibited the highest catalytic activity, which is attributed to the bimolecular activation channels formed by metal nanoparticles and Ti3C2Tx-Y.