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通过动态核极化增强核磁共振观察碳酸钙的瞬态预成核物种

Observation of Transient Prenucleation Species of Calcium Carbonate by DNP-Enhanced NMR.

作者信息

Balodis Martins, Rao Yu, Stevanato Gabriele, Kellner Matthias, Meibom Josephine, Negroni Mattia, Chmelka Bradley F, Emsley Lyndon

机构信息

Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland.

Department of Chemical Engineering, University of California, Santa Barbara, California 93106-5080, United States.

出版信息

J Phys Chem Lett. 2024 Aug 8;15(31):7954-7961. doi: 10.1021/acs.jpclett.4c01588. Epub 2024 Jul 29.

Abstract

Knowledge of the mechanism by which polymorphic inorganic species, such as carbonates, are formed is crucial to understand and guide the selective crystallization of end products. Recently it has been shown that a key step in the crystallization of calcium carbonate is the formation of intermediate species known as prenucleation clusters. However, the observation of these prenucleation clusters in solution is exceedingly challenging because of their short lifetime and low concentrations. Here, using dissolution DNP-enhanced NMR spectroscopy, we observe signals from prenucleation species of calcium carbonate from which the kinetics of formation and conversion are determined.

摘要

了解多晶型无机物种(如碳酸盐)的形成机制对于理解和指导最终产物的选择性结晶至关重要。最近有研究表明,碳酸钙结晶的一个关键步骤是形成称为预成核簇的中间物种。然而,由于这些预成核簇的寿命短且浓度低,在溶液中观察它们极具挑战性。在这里,我们使用溶解态动态核极化增强核磁共振光谱法,观察到了碳酸钙预成核物种的信号,并由此确定了其形成和转化的动力学。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cb3f/11318035/6c43394c2b68/jz4c01588_0001.jpg

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