层状多孔炭片负载钌催化剂的制备及其催化氨硼烷水解制氢性能研究

Preparation of layered porous carbon supported ruthenium catalyst and its performance for ammonia borane hydrolyzing to hydrogen

  • 摘要: 本研究以煤沥青为炭材料,氯化钠为模板剂,碳酸钾为活化剂,在氩气气氛下高温煅烧得到载体层状多孔炭片(LPCS),通过浸渍法向其中加入RuCl3金属溶液,将活性组分Ru负载到LPCS载体上合成Ru/LPCS催化剂,并对其催化氨硼烷水解制氢的性能进行了研究。结果表明,Ru/LPCS催化剂中,当煅烧温度为1123 K时,Ru的负载量为2%时,催化剂的反应转化频率(TOF)值最大,此时有光下催化剂的TOF为334.8 min−1,是无光照时TOF的1.38倍。在光照下,催化剂的活化能(Ea)从90.60 kJ/mol下降到70.33 kJ/mol。氨硼烷水解制氢速率相对于其浓度的级数为0.75,而相对于催化剂的用量满足于一级动力学关系。

     

    Abstract: In this paper, layered porous carbon sheet (LPCS) was obtained through high temperature calcination under argon atmosphere by using coal pitch as carbon material, sodium chloride as template agent and potassium carbonate as activator. Then, the active component Ru was loaded onto the LPCS support by impregnation to synthesize Ru/LPCS catalyst whose catalytic performance for hydrogen production by hydrolysis of ammonia borane was studied. The results showed that in the presence of light, the maximum value of the turnover frequency (TOF), 334.8 min−1, was obtained at a calcination temperature of 1123 K and a loading of 2% of Ru which is 1.38 times higher than that in the absence of light. The activation energy (Ea) of the catalyst decreased from 90.60 to 70.33 kJ/mol in the presence of light. The hydrogen production rate order with respect to ammonia borane concentration was 0.75, which is first-order relation to the amount of the catalyst.

     

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