Comparative study of alumina-supported transition metal catalysts for hydrogen generation by steam reforming of acetic acid
Comparative study of alumina-supported transition metal catalysts for hydrogen generation by steam reforming of acetic acid
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DOI：
10.1016/j.apcatb.2010.06.035
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发表时间：
2010-08
影响因子：
22.1
通讯作者：
Xun Hu;Gongxuan Lu
中科院分区：
文献类型：
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作者：
Xun Hu;Gongxuan Lu
研究了过渡金属（Ni、Co、Fe和Cu）/Al_2O_3催化剂上乙酸水蒸气重整制氢反应。Ni/Al_2O_3和Co/Al_2O_3催化剂对乙酸水蒸气重整反应具有较好的活性，而Fe/Al_2O_3和Cu/Al_2O_3催化剂的活性较低。这种差异是由于金属对乙酸分子中C-C和C-H键的裂解活性不同。详细比较了Ni/Al_2O_3和Co/Al_2O_3催化剂的催化活性、选择性和稳定性。在它们之间观察到不同的产物分布。Ni/Al 2 O3催化剂在温和温度下有利于CH 4的生成，而Co/Al 2 O3催化剂在高温下有利于CO的生成，这是由两种催化剂上不同的反应网络引起的。此外，在稳定性试验中，Ni/Al 2 O3催化剂比Co/Al 2 O3催化剂稳定得多。Co/Al 2 O3催化剂的失活主要是由于积炭和金属相的氧化。相反，Ni/Al_2O_3催化剂的积炭速率和金属烧结速率明显降低，活性金属的抗氧化性明显提高，从而保证了催化剂的稳定性。
The reaction of acetic acid steam reforming for H2production has been investigated over transition metal catalysts (Ni, Co, Fe or Cu)/Al2O3. Ni/Al2O3and Co/Al2O3catalysts are active for acetic acid steam reforming while Fe/Al2O3and Cu/Al2O3catalysts present negligible activity. The difference can be attributed to the different cracking activity of the metals toward the C–C and C–H bonds of acetic acid molecule. Detailed comparisons in terms of catalytic activity, selectivity, and stability are carried out over Ni/Al2O3and Co/Al2O3catalysts. Distinct product distributions were observed between them. CH4production was favored over Ni/Al2O3catalyst at mild temperatures while CO production was favored over Co/Al2O3catalyst at high temperatures, which were induced by the different reaction networks over the two catalysts. Moreover, in the stability tests, Ni/Al2O3catalyst was much more stable than Co/Al2O3catalyst. Serious coke deposition and oxidation of metallic phase led to the fast deactivation of Co/Al2O3catalyst. On the contrary, much slower coke formation rates and metal sintering rates as well as much higher resistivity of active metal toward oxidation guaranteed the stability of Ni/Al2O3catalyst.