Dual catalytic activity of a cucurbit[7]uril-functionalized metal alloy nanocomposite for sustained hydrogen generation: hydrolysis of ammonia borane and electrocatalysts for the hydrogen evolution reaction.

H 2 is one of the most attractive fuel alternatives to the existing fossil fuels that cause detrimental environmental issues. Thus, there has been an upsurge in the research on the production of green hydrogen. In this view, cucurbit[7]uril (CB7)-functionalized Co:Ni alloy nanocomposites with different compositions, reported here for the first time, were synthesized to synergise the catalytic activities of a nanoalloy and CB7 and screened for hydrogen generation via hydrolysis of ammonia borane (AB). The (Co 85 :Ni 15 ) 50 :(CB7) 50 nanocomposite exhibited enhanced catalytic performance for AB hydrolysis even at room temperature as compared to the nanoalloy without CB7. Efficient release of ammonia-free green H 2 is ensured by the retention of NH 3 by the surface functionalized CB7 macrocycles. For sustained release, a novel and cost-effective procedure was used to regenerate AB from the by-product, and the H 2 release activity was verified to be on par with commercial AB. The used nanocomposite magnetically separated from the by-product solution was shown to be an efficient electrochemical catalyst for the hydrogen evolution reaction (HER). The cucurbit[7]uril-functionalized Co:Ni nanocomposite demonstrates remarkable dual catalytic performance to generate clean hydrogen from both the hydrolysis of AB at room temperature and the electrochemical HER, thus opening new avenues in supramolecular chemistry for developing noble metal-free catalysts with high activity and long-term stability.