Designing Metal‐Free Frustrated Lewis Pairs Catalyst for the Efficient Dehydrogenation of Ammonia Borane. Issue 50 (3rd August 2018)

• Record Type: Journal Article
• Authors: Ma, Gongli; Song, Guoliang; Li, Zhen Hua
• Is Part Of: Chemistry. Volume 24:Issue 50(2018)
• Page Start: 13238
• Page End: 13245
• Publication Date: 2018-08-03
• Subjects: ammonia borane -- boranes -- chemical hydrogen storage -- density functional calculations -- frustrated Lewis pairs -- kinetic Monte Carlo -- metal-free catalysis; Chemistry -- Periodicals; 540
• DOI: 10.1002/chem.201801932
• Languages: English
• ISSNs: 0947-6539

Abstract

Abstract: Ammonia borane (AB ) has been in the spotlight for the chemical storage of hydrogen over the past decade. However, the development of methods for efficient and controlled hydrogen release fromAB under mild conditions is still underway. Herein, using density functional theory (DFT) computations, we designed a metal‐free frustrated Lewis pair (FLP) catalyst o ‐(BPh2 )C6 H4 (N i Pr2 ) (M1 ) that can efficiently dehydrogenateAB to release more than two equivalents of H2 under mild conditions. CatalystM1 can dehydrogenate not onlyAB to H2 N=BH2 (AOB ) and H2, but also oligomers ofAOB with rather low free‐energy barriers. The high dehydrogenation activity ofM1 is the key of new oligomerization routes to the efficient dehydrogenation ofAB to borazine (BZ ) or H2 B−(NH=BH) n −NH2 (PIB ) and finally to polyborazylene (PBZ ) so that more than two equivalents of H2 can be released. A first‐principle kinetic Monte Carlo (KMC) study reveals that the activity of our catalytic system can be tuned by varying the initial concentration ofM1 andAB . This work can guide the design of catalyst for the highly efficient utilization ofAB as a hydrogen storage material. Abstract : Novel dehydrogenation strategy : With the help of accurate theoretical methods, a metal‐free frustrated Lewis pair (FLP) catalyst o ‐(BPh2 )C6 H4 (N i Pr2 ) (M1 ) was designed that can efficiently dehydrogenate ammonia borane (AB ) to controllably release more than two equivalents of H2 under mild conditions.