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Studies On The Hydrolytic Dehyrogenation Of Amine Borane By Transition Metal Iron,Cobalt And Nickel Nanoparticle

Posted on:2020-10-21Degree:MasterType:Thesis
Country:ChinaCandidate:K X ZhangFull Text:PDF
GTID:2381330578467948Subject:Chemistry
Abstract/Summary:PDF Full Text Request
Hydrogen is currently considered one of the cleanest and most sustainable sources of energy compared to the use of coal,oil,and natural gas as a source of energy to cause air pollution and the greenhouse effect.However,hydrogen energy fuel: hydrogen,its transportation is one of the main reasons for the delay of hydrogen energy development.Borane-nitrogen-hydrogen(B-N-H)compounds generally have high hydrogen storage density and have great potential in transport applications.Ammonia borane(AB)is the simplest B-N-H compounds.It is stabilized at normal temperature and pressure,and it is solid.In addition,ammonia borane can release three equivalents of hydrogen at most,and it have high hydrogen content(19.6 %),which is a very ideal material for storage and transportation.Therefore,in this work we devoted to development Fe,Co,and Ni nanoparticles as catalyst to release hydrogen from ammonia borane,N-methylamine borane(Me AB)and N,N-dimethylamine borane(Me2AB).First,we successfully synthesized a series of metal nanoparticle using tetrahydrofuran borane as a reducing agent,Fe NPs,Co NPs,Ni NPs,Fe/ZIF-8 NPs,Co/ZIF-8 NPs and Ni/ZIF-8 NPs,which were characterized by XRD,SEM,TEM,XPS.Second,we have found that they all efficiently catalyze the hydrolysis of ammonia borane to release hydrogen.The TOF of ammonia borane catalyzed by Fe NPs,Co NPs,Ni NPs,Co/ZIF-8 NPs and Ni/ZIF-8 NPs were 26.2 min-1,82.7 min-1,81.8 min-1,54.6 min-1,66.2 min-1 respectively.In addition,Ni NPs and Co/ZIF-8 NPs also have high catalytic properties for methylamine borane and dimethylamine borane,enabling them to hydrolyze completely,of which the TOF of Ni NPs catalyzed hydrolysis of methylamine borane and dimethylamine borane were 44.1 min-1 and 23.7 min-1.The TOF of Co/ZIF-8 NPs catalyzed hydrolysis of methylamine borane and dimethylamine borane were 26.3 min-1,21.7 min-1.The results of this research have important implications for the subsequent development of amine borane heterogeneous catalysts.We have successfully simplified the method of synthesizing aminodiborane(ADB),and attempts to use aminodiboranes with different substituents to react with a series of amines to obtain a new series of small molecular chain borane-nitrogen-hydrogen compounds,the structure is determined by NMR.The related reaction mechanism and catalytic hydrogen production reaction need further research and discuss.
Keywords/Search Tags:borane-nitrogen-hydrogen compounds, tetrahydrofuran borane, nanoparticles, amine borane, hydrolysis
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