Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany.
Physical Chemistry, Department of Chemistry, University of Konstanz, Universitätsstrasse 10, Konstanz 78464, Germany.
J Am Chem Soc. 2021 Feb 3;143(4):1758-1762. doi: 10.1021/jacs.0c11976. Epub 2021 Jan 20.
Biomineralization occurs in aqueous environments. Despite the ubiquity and relevance of CaCO biomineralization, the role of water in the biomineralization process has remained elusive. Here, we demonstrate that water reorganization accompanies CaCO biomineralization for sea urchin spine generation in a model system. Using surface-specific vibrational spectroscopy, we probe the water at the interface of the spine-associated protein during CaCO mineralization. Our results show that, while the protein structure remains unchanged, the structure of interfacial water is perturbed differently in the presence of both Ca and CO compared to the addition of only Ca. This difference is attributed to the condensation of prenucleation mineral species. Our findings are consistent with a nonclassical mineralization pathway for sea urchin spine generation and highlight the importance of protein hydration in biomineralization.
生物矿化发生在水相环境中。尽管 CaCO 生物矿化无处不在且具有重要意义，但水在生物矿化过程中的作用仍然难以捉摸。在这里，我们在一个模型系统中证明了水的重组伴随着海胆刺生成过程中的 CaCO 生物矿化。我们使用表面特定的振动光谱技术，在 CaCO 矿化过程中探测与刺相关的蛋白质界面处的水。我们的结果表明，虽然蛋白质结构保持不变，但与仅添加 Ca 相比，在存在 Ca 和 CO 的情况下，界面水的结构受到不同的干扰。这种差异归因于成核前矿物物种的缩合。我们的发现与海胆刺生成的非经典矿化途径一致，并强调了蛋白质水合在生物矿化中的重要性。
