Bottom-Up Self-Assembly of Amorphous Core–Shell–Shell Nanoparticles and Biomimetic Crystal Forms in Inorganic Silica–Carbonate Systems
Bottom-Up Self-Assembly of Amorphous Core–Shell–Shell Nanoparticles and Biomimetic Crystal Forms in Inorganic Silica–Carbonate Systems
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DOI：
10.1021/cm4003959
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发表时间：
2013-04
影响因子：
8.6
通讯作者：
J. Eiblmeier;M. Kellermeier;M. Deng;L. Kienle;J. G. Ruiz;W. Kunz
中科院分区：
文献类型：
--
作者：
J. Eiblmeier;M. Kellermeier;M. Deng;L. Kienle;J. G. Ruiz;W. Kunz
碱土碳酸盐在高pH值富硅介质中的矿化作用导致了迷人的晶体形态，尽管没有任何有机物，但这些晶体形态与生物矿化的产物非常相似。最近的研究表明，即使在高过饱和度的情况下，也可以在这样的体系中生长出精细的CaCO3结构，因为无定形碳酸钙(ACC)的纳米颗粒自发地被二氧化硅表面包裹，从而作为临时储存库，不断地为结晶方解石的形成提供生长单元。在目前的研究中，我们在类似的条件下沉淀了碳酸钡，发现了令人惊讶的不同行为。在低二氧化硅浓度下，由于硅酸盐低聚物对生长过程的毒害影响，没有证据表明存在无定形碳酸盐前驱物，立即发生晶化，导致细长晶体表现出渐进的自相似分支。在硅胶中超过一定的阈值。
Mineralization of alkaline-earth carbonates in silica-rich media at high pH leads to fascinating crystal morphologies that strongly resemble products from biomineralization, despite the absence of any organic matter. Recent work has demonstrated that elaborate CaCO3 structures can be grown in such systems even at high supersaturation, as nanoparticles of amorphous calcium carbonate (ACC) were spontaneously coated by skins of silica and thus served as temporary storage depots continuously supplying growth units for the formation of crystalline calcite. In the present study, we have precipitated barium carbonate under similar conditions and found surprisingly different behavior. At low silica concentrations, there was no evidence for an amorphous carbonate precursor phase and crystallization occurred immediately, resulting in elongated crystals that showed progressive self-similar branching due to the poisoning influence of silicate oligomers on the growth process. Above a certain threshold in the silica co...