Hydrogen production by steam reforming of acetic acid: Comparison of conventional supported metal catalysts and metal-incorporated mesoporous smectite-like catalysts

Hydrogen production by steam reforming of acetic acid: Comparison of conventional supported metal catalysts and metal-incorporated mesoporous smectite-like catalysts
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乙酸蒸汽重整制氢:传统负载型金属催化剂和金属掺入的介孔蒙脱石催化剂的比较

DOI:
10.1016/j.ijhydene.2009.10.053
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发表时间:
2010
期刊:
影响因子:
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通讯作者:
Masahiko Arai
Masahiko Arai
中科院分区:
--
文献类型:
--
作者:
N. Iwasa;Toshiyuki Yamane;Masaaki Takei;Jun;Masahiko Arai

文献摘要

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以传统的金属氧化物和过渡金属掺杂的中孔蒙脱石类材料为载体,考察了不同金属催化剂在乙酸水蒸气重整制氢反应中的活性。结果表明,在Al_2O_3负载型催化剂中,Pt比Ni、Co和Fe具有上级的催化活性,Al_2O_3比ZrO_2和SiO_2更适合于Pt的负载,Ni掺杂的蒙脱石(SM(Ni))比Fe和Co掺杂的蒙脱石更适合于Pt的负载,SM(Ni)在不含Pt的情况下也具有活性。催化剂对乙酸的总转化活性为Pt/Al_2 O_3>Pt/SM(Ni)>SM(Ni),但产氢能力相当。观察到这些催化剂(和其它催化剂)在重整反应期间失去其活性。Pt/Al_2O_3催化剂的活性在整个反应过程中一直下降,直至10 h。而SM(Ni)的活性在2 h内也有所下降,但在反应后期表现出稳定的活性。使用的Pt/SM(Ni)和SM(Ni)的初始活性能够通过用H2热处理而几乎完全恢复,但对于使用的Pt/Al 2 O3不太有效。催化剂失活的发生是由碳材料在催化剂上的形成和沉积(XRD,TEM,热分析)。Pt/Al_2 O_3和SM(Ni)催化剂上积炭的性质不同,这可能是导致两种催化剂失活程度和再生行为不同的原因。
The activities of various metal catalysts were tested in steam reforming of acetic acid for the production of H2, using conventional metal oxides and transition metal-incorporated mesoporous smectite-like materials as supports. It has been found that Pt is superior to Ni, Co, and Fe among Al2O3supported catalysts, Al2O3is more effective than ZrO2and SiO2as support for Pt, Ni incorporated smectite (SM(Ni)) support is more effective than Fe and Co incorporated ones for Pt, and SM(Ni) is also active in the absence of Pt. The total activity for the conversion of acetic acid is in the order of Pt/Al2O3>Pt/SM(Ni)>SM(Ni) but the ability of H2production is comparable among these catalysts. These catalysts (and the other ones) were observed to lose their activities during the reforming reactions. The activity of Pt/Al2O3decreased during the whole course of reaction up to 10h. In contrast, the activity of SM(Ni) also decreased within 2h but it showed a stable activity in the following stage of reaction. The initial activity of the used Pt/SM(Ni) and SM(Ni) was able to be almost completely restored by thermal treatment with H2but less effectively for the used Pt/Al2O3. The catalyst deactivation was shown to occur by the formation and deposition of carbon materials on the catalysts (XRD, TEM, thermal analysis). The properties of carbon deposits formed on Pt/Al2O3and SM(Ni) catalysts should be different and this may be responsible for the differences in the extent of deactivation and in the regeneration behavior between the two catalysts.