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Lookup NU author(s): Dr Corinne Wills, Dr Casey Dixon, Dr Elisabetta Arca, Dr Julian Knight, Dr Simon DohertyORCiD
This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).
Platinum and ruthenium nanoparticles stabilised by an amine modified polymer immobilised ionic liquid (MNP@NH2-PEGPIILS, M = Pt, Ru) catalyse the hydrolytic liberation of hydrogen from dimethylamine borane (DMAB), amine borane (AB) and NaBH4 under mild conditions. While RuNP@NH2-PEGPIILS and PtNP@NH2-PEGPIILS catalyse the hydrolytic evolution of hydrogen from NaBH4 with comparable initial TOFs of 6,200 and 5,900 molesH2.molcat-1.min-1, respectively, RuNP@NH2-PEGPIILS is a markedly more efficient catalyst for the dehydrogenation of DMAB and AB than its platinum counterpart, as RuNP@NH2-PEGPIILS gave initial TOFs of 8,050 molesH2.molcat-1.min-1 and 21,200 molesH2.molcat-1.min-1, respectively, compared with 3,050 molesH2.molcat-1.min-1 and 8,500 molesH2.molcat-1.min-1, respectively, for PtNP@NH2-PEGPIILS. Gratifyingly, for each substrate tested RuNP@NH2-PEGPIILS and PtNP@NH2-PEGPIILS were markedly more active than commercial 5wt % Ru/C and 5wt% Pt/C, respectively. The apparent activation energies of 55.7 kJ mol-1 and 27.9 kJ mol-1 for the catalytic hydrolysis of DMAB and AB, respectively, with RuNP@NH2-PEGPIILS are significantly lower than the respective activation energies of 74.6 kJ mol-1 and 35.7 kJ mol-1 for its platinum counterpart, commensurate with the markedly higher initial rates obtained with the RuNPs. In comparison, the apparent activation energies of 44.1 kJ mol-1 and 46.5 kJ mol-1, for the hydrolysis NaBH4 reflect the similar initial TOFs obtained for both catalysts. The difference in apparent activation energies for the hydrolysis of DMAB compared with AB also reflect the higher rates of hydrolysis for the latter. Stability and reuse studies revealed that RuNP@NH2-PEGPIILS recycled efficiently as high conversions for the hydrolysis of DMAB were maintained across five runs with the catalyst retaining 97% of its activity.
Author(s): Alharbi AA, Wills C, Dixon C, Chamberlain T, Arca E, Griffiths A, Collins S, Wu K, Yan H, Bourne R, Knight J, Doherty S
Publication type: Article
Publication status: Published
Journal: Catalysis Letters
Year: 2024
Volume: 154
Pages: 5450–5471
Print publication date: 01/10/2024
Online publication date: 04/06/2024
Acceptance date: 23/05/2024
Date deposited: 23/05/2024
ISSN (print): 1011-372X
ISSN (electronic): 1572-879X
Publisher: Springer Nature
URL: https://doi.org/10.1007/s10562-024-04725-8
DOI: 10.1007/s10562-024-04725-8
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