Karel Frolich , Jan Malina , Martin Hájek , Jaroslav Kocík
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引用次数: 0
摘要
生物乙醇选择性催化转化为有价值的化合物,尤其是 1-丁醇(即格贝特反应),因其在未来替代化石能源的潜力而备受关注。这项研究继续寻找一种具有高乙醇转化率和对所需产品选择性的催化剂。这项研究的新颖之处在于使用铜-锂-铝混合金属氧化物作为异相催化剂。锂铝氧化物通过尿素沉淀制备,铜通过两种方式引入:(i) 共沉淀和 (ii) 合成后浸渍。在不同温度和压力下,在固定床反应器中实现了气相反应。事实证明,混合金属氧化物的特性至关重要,因为可以观察到多种产品。催化剂从酸性转变为碱性,以及具有不同氧化还原特性,都会显著影响乙醇转化率和对所需高级醇的选择性。与之前使用的镁铝混合金属氧化物相比,在 300-350 °C 和 10 兆帕条件下,只需较低量的铜即可实现类似或更高的乙醇转化率(71%)和丁醇选择性(30%)。因此,锂铝混合金属氧化物显示出超越镁铝混合金属氧化物的潜力,只需进一步研究和调整其特性即可。
The utilization of ethanol for production of 1-butanol catalysed by Li–Al mixed metal oxides enhanced by Cu
The selective catalytic conversion of bio-ethanol into valuable chemical compounds, particularly 1-butanol (i.e., Guerbet reaction), has gained significant attention due to its potential to replace fossil sources in the future. This work continues the search for a catalyst with high ethanol conversion and selectivity toward desired products. The novelty of the study lies in its use of copper-lithium-aluminum mixed metal oxides as heterogeneous catalysts. Li–Al oxides were prepared via urea precipitation, and copper was introduced in two ways: (i) during co-precipitation and (ii) post-synthetic impregnation. Gas-phase reaction in a fixed-bed reactor was realized at varying temperatures and pressures. The properties of the mixed metal oxides proved to be crucial, as a wide range of products was observed. Catalysts that shifted from acidic to basic properties, and those with different redox properties, significantly affected ethanol conversion and selectivity toward the desired higher alcohols. Compared to previously used magnesium-aluminum mixed metal oxides, a lower amount of copper was required to achieve similar or higher ethanol conversion (71 %) and butanol selectivity (30 %) at 300–350 °C and 10 MPa. Thus, lithium-aluminum mixed metal oxides showed the potential to surpass magnesium-aluminum mixed metal oxides with further study and adjustment of their properties.
期刊介绍:
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