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Utilization of Liquid Organic Hydrides for Hydrogen Storage and Supplyto Fuel Cells. Efficient Hydrogen Supply by the Spray-Pulse ModeReactors with Cyclohexane, Decalin

机译:利用液态有机氢化物储存氢并供应给燃料电池。带有环己烷,十氢化萘的喷雾脉冲反应器可有效供应氢气

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By use of the several kinds of spray-pulse reactors, highly efficient production of hydrogenwithout CO2 emission by the dehydrogenation of liquid organic hydrides (cyclohexane,methylcyclohexane, cis-decalin, trans-decalin, 1-methylcyclohexane, cyclohexylbenzene,bicyclohexyl) is achieved at 220 - 400 ℃ on the carbon-supported Pt-containing catalysts(Pt/AC, Pt-M/AC, where M = Re, Rh, Pd, or Ir). In the fundamental studies with small-scalereactors (500 mL and 2000 mL), it is revealed that the efficiency of hydrogen evolutiondepends on support, reactant, loading of catalyst, reaction temperature, and the spray size andpulse interval of the reactor. The rates of dehydrogenation were in the following order:cyclohexylbenzene > cyclohexane, methylcyclohexane, bicyclohexyl > cis-decalin,1-methyldecalin > trans-decalin. Comparing the reactants, the highest reaction rate wasobserved for cyclohexylbenzene. The highest hydrogen production rate (110 mL min -1 ) wasobserved for bicyclohexyl, due to its high hydrogen contents in a molecule. ComparingPt/AC and Pt-M/AC, Pt-Rh/AC bimetallic catalysts showed higher activities fordehydrogenation of cyclohexane, due to the electronic effect of these second metals.Comparing the cis-decalin and trans-decalin, cis- isomer showed higher reaction rate thantrans- isomer, reflecting the difference of free energy (?G) between the product (naphthalene)and the reactants. Several types of spray-pulse reactors have provided the demonstrations ofthe fuel cell operation by dehydrogenation of cyclohexane and decalin.
机译:通过使用几种喷雾脉冲反应器,可以在液态有机氢化物(环己烷,甲基环己烷,顺式十氢萘,反式十氢萘,1-甲基环己烷,环己基苯,双环己基)脱氢的情况下高效生产氢气而不会产生CO2排放。碳负载的含Pt催化剂(Pt / AC,Pt-M / AC,其中M = Re,Rh,Pd或Ir)在220-400℃上。在使用小型反应器(500 mL和2000 mL)的基础研究中,发现氢气的释放效率取决于载体,反应物,催化剂的负载量,反应温度以及反应器的喷雾尺寸和脉冲间隔。脱氢速率按以下顺序:环己基苯>环己烷,甲基环己烷,双环己基>顺式十氢化萘,1-甲基十氢化萘>反式十氢化萘。比较反应物,环己基苯的反应速率最高。由于双环己基在分子中的氢含量高,因此观察到最高的氢生产率(110 mL min -1)。比较Pt / AC和Pt-M / AC,由于这些第二种金属的电子效应,Pt-Rh / AC双金属催化剂显示出更高的环己烷脱氢活性。对比顺式十氢化萘和反式十氢化萘,顺式异构体显示出更高的反应速率高于反式异构体,反映出产物(萘)和反应物之间的自由能(ΔG)之差。几种类型的喷雾脉冲反应器通过环己烷和十氢化萘的脱氢提供了燃料电池运行的演示。

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