Deep eutectic-solvothermal synthesis of nanostructured ceria.
Deep eutectic-solvothermal synthesis of nanostructured ceria.
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DOI：
10.1038/ncomms14150
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发表时间：
2017-01-25
影响因子：
16.6
通讯作者：
Torrente-Murciano L
中科院分区：
文献类型：
--
作者：
Hammond OS;Edler KJ;Bowron DT;Torrente-Murciano L
二氧化铈是一种技术上重要的材料，在催化、排放控制和固体氧化物燃料电池中都有应用。纳米结构的氧化铈由于其提高的表面积体积比、活性表面氧空位浓度和优异的储氧能力而变得更加活跃。在这里，我们报告了使用绿色深共晶溶剂线合成纳米结构的二氧化铈，这使得形貌和孔隙度控制成为迄今为止报道的低能耗路线之一。利用宽q范围液相中子衍射，我们在分子尺度上阐明了反应机理，其条件比传统的水热合成路线温和得多。线溶剂起着潜在超分子催化剂的作用，其中由溶剂驱动的反应物预组织的反应速率的增加是最显著的。这种对深度共晶-溶剂热方法的基本理解将促进纳米结构二氧化铈低温合成的未来发展，促进其使用绿色、经济、无毒溶剂的大规模生产。在绿色深共晶溶剂线上合成纳米结构的二氧化铈是迄今为止能源消耗较低的方法之一。在这里，作者表明，线溶剂起着潜在的超分子催化剂的作用，驱动反应物的预组织，允许形貌和孔隙度控制。
Ceria is a technologically important material with applications in catalysis, emissions control and solid-oxide fuel cells. Nanostructured ceria becomes profoundly more active due to its enhanced surface area to volume ratio, reactive surface oxygen vacancy concentration and superior oxygen storage capacity. Here we report the synthesis of nanostructured ceria using the green Deep Eutectic Solvent reline, which allows morphology and porosity control in one of the less energy-intensive routes reported to date. Using wide Q-range liquid-phase neutron diffraction, we elucidate the mechanism of reaction at a molecular scale at considerably milder conditions than the conventional hydrothermal synthetic routes. The reline solvent plays the role of a latent supramolecular catalyst where the increase in reaction rate from solvent-driven pre-organization of the reactants is most significant. This fundamental understanding of deep eutectic-solvothermal methodology will enable future developments in low-temperature synthesis of nanostructured ceria, facilitating its large-scale manufacturing using green, economic, non-toxic solvents. Synthesis of nanostructured ceria on green deep eutectic solvent reline is one of the less energy-intensive routes to date. Here, the authors show that the reline solvent plays the role of a latent supramolecular catalyst driving the pre-organization of the reactants, allowing morphology and porosity control.