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Triethylamine–Water as a Switchable Solvent for the Synthesis of Cu/ZnO Catalysts for Carbon Dioxide Hydrogenation to Methanol
Topics in Catalysis ( IF 2.8 ) Pub Date : 2021-06-12 , DOI: 10.1007/s11244-021-01457-6
William T. Wallace , James S. Hayward , Chen-Yu Ho , Amy R. Marsh , Anisa Tariq , Jonathan K. Bartley

Cu/ZnO catalyst precursors for industrial methanol synthesis catalysts are traditionally synthesised by coprecipitation. In this study, a new precipitation route has been investigated based on anti-solvent precipitation using a switchable solvent system of triethylamine and water. This system forms a biphasic system under a nitrogen atmosphere and can be switched to an ionic liquid single phase under a carbon dioxide atmosphere. When metal nitrate solutions were precipitated from water using triethylamine–water as the anti-solvent a hydroxynitrate phase, gerhardite, was formed, rather than the hydroxycarbonate, malachite, formed by coprecipitation. When calcined and reduced, the gerhardite precursors formed Cu/ZnO catalysts which showed better productivity for methanol synthesis from CO2 hydrogenation than a traditional malachite precursor, despite their larger CuO crystallite size determined by X-ray diffraction. The solvents could be recovered by switching to the biphasic system after precipitation, to allow solvent recycling in the process, reducing waste associated with the catalyst synthesis.



中文翻译:

三乙胺-水作为可转换溶剂合成用于二氧化碳加氢制甲醇的 Cu/ZnO 催化剂

用于工业甲醇合成催化剂的 Cu/ZnO 催化剂前体传统上是通过共沉淀法合成的。在这项研究中,基于使用三乙胺和水的可转换溶剂系统的反溶剂沉淀,研究了一种新的沉淀路线。该体系在氮气氛下形成双相体系,在二氧化碳气氛下可转变为离子液体单相。当使用三乙胺-水作为反溶剂从水中沉淀出金属硝酸盐溶液时,会形成羟基硝酸盐相,即gerhardite,而不是通过共沉淀形成的羟基碳酸盐,孔雀石。当煅烧和还原时,黄铜矿前驱体形成了 Cu/ZnO 催化剂,显示出更好的从 CO 2合成甲醇的生产率尽管 X 射线衍射测定的 CuO 微晶尺寸更大,但与传统的孔雀石前驱体相比,氢化反应更明显。可以通过在沉淀后切换到双相系统来回收溶剂,以便在过程中回收溶剂,减少与催化剂合成相关的浪费。

更新日期:2021-06-13
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