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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Pressure-regulated synthesis of Cu(TPA)center dot(DMF) in microdroplets for selective CO2 adsorption
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Pressure-regulated synthesis of Cu(TPA)center dot(DMF) in microdroplets for selective CO2 adsorption

机译：用于选择性CO2吸附的微量滴水中Cu（TPA）中心点（DMF）的压力调节合成

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The synthesis of metal-organic frameworks (MOFs) by using traditional wet-chemistry methods generally requires very long durations and still suffers from non-uniform heat and mass transfer within the bulk precursor solutions. Towards addressing these issues, a microdroplet-based spray method has been developed. In a typical spray process, an MOF's precursor solution is first atomized into microdroplets. These droplets serve as microreactors to ensure homogeneous mixing, fast evaporation, and rapid nucleation and crystal growth to form MOF particles. However, the fundamental MOF formation mechanisms by using this strategy have not been fully understood. In this work, the role of the operating pressure in the synthesis of a representative MOF (i.e., Cu(TPA) center dot (DMF); TPA: terephthalic acid, DMF: dimethylformamide) was systematically investigated. Detailed characterization showed that the pressure variations significantly affected both the morphologies and crystalline structures of Cu(TPA) center dot (DMF). Numerical simulations revealed that the morphology changes are mainly attributed to the variations in supersaturation ratios, which are caused by different microdroplet evaporation rates due to the regulation of operating pressure, while the crystalline structure variations are closely related to the dissociation of DMF molecules at lower operating pressures. Besides, the dissociation of DMF molecules decreased the surface area of the MOF crystals, but gave rise to massive coordinatively unsaturated metal sites, which greatly enhanced the interaction of CO2 with the MOF crystal and thus led to improved CO2 adsorption capacity and selectivity. The outcome of this work would contribute to the fundamental understanding of MOF synthesis using the microdroplet-based spray method.
机译：通过使用传统的湿化学方法合成金属 - 有机骨架（MOF）通常需要非常长的持续时间，并且仍然存在在本体前体溶液中的不均匀的热量和传质。在解决这些问题方面，已经开发了一种基于Microdroplet的喷射方法。在典型的喷雾过程中，首先将MOF的前体溶液雾化成微量滴电池。这些液滴用作微反应器，以确保均匀混合，快速蒸发和快速成核和晶体生长以形成MOF颗粒。然而，使用这种策略的基本MOF形成机制尚未得到完全理解。在这项工作中，系统地研究了在合成代表性MOF的合成中的作用（即Cu（TPA）中心点（DMF）; TPA：对苯二甲酸，DMF：二甲基甲酰胺）的作用。详细表征显示压力变化显着影响Cu（TPA）中心点（DMF）的形态和结晶结构。数值模拟显示，形态变化主要归因于超饱和度比的变化，这是由于由于操作压力的调节而引起的不同的微滴蒸发速率，而结晶结构变化与DMF分子的解离在较低操作下的解离相关压力。此外，DMF分子的解离降低了MOF晶体的表面积，但是产生了巨大的坐标不饱和金属位点，这大大提高了CO 2与MOF晶体的相互作用，从而提高了CO 2吸附能力和选择性。该工作的结果将有助于使用基于Microdroplet的喷雾方法对MOF合成的基本理解。

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