Reaction mechanism and kinetics for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst
Journal article, Peer reviewed
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OriginalversjonAIChE Journal. 2017, 63 (1), 60-65. 10.1002/aic.15389
A reaction mechanism is proposed for hydrolytic dehydrogenation of ammonia borane on a Pt/CNT catalyst. A combination of thermodynamic analysis and FTIR measurement reveals that B‐containing byproducts are mainly in the form of an NH4B(OH)4‐B(OH)3 mixture rather than NH4BO2 reported previously. The revised main reaction is urn:x-wiley:00011541:media:aic15389:aic15389-math-0001, involving the B–H, B–N, and O–H bond cleavages. Isotopic experiments using D2O instead of H2O as reactant or introducing D2 into the reaction atmosphere suggest the O–H bond cleavage being in the rate‐determining step, and an unfavorable occurrence of the chemisorbed H2O dissociation (i.e., the direct O–H bond cleavage), respectively. Different reaction pathways with indirect O–H bond cleavages are analyzed, and then urn:x-wiley:00011541:media:aic15389:aic15389-math-0002 is suggested as the rate‐determining step. Subsequently, a Langmuir–Hinshelwood kinetic model is developed, which fits well with the experimental data.