State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;; Department of Chemistry and Biochemistry, Jackson State University, Jackson, MS 39203, USA;
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China;
Regen Biomater. 2015 Sep;2(3):187-95. doi: 10.1093/rb/rbv010. Epub 2015 Aug 17.
Four self-assembled monolayer surfaces terminated with -COOH, -OH, -NH2 and -CH3 functional groups are used to direct the biomineralization processes of calcium carbonate (CaCO3) in low Ca(2+) concentration, and the mechanism of nucleation and initial crystallization within 12 h was further explored. On -COOH surface, nucleation occurs mainly via ion aggregation mechanism while prenucleation ions clusters may be also involved. On -OH and -NH2 surfaces, however, nucleation forms via calcium carbonate clusters, which aggregate in solution and then are adsorbed onto surfaces following with nucleation of amorphous calcium carbonate (ACC). Furthermore, strongly negative-charged -COOH surface facilitates the direct formation of calcites, and the -OH and -NH2 surfaces determine the formation of vaterites with preferred crystalline orientations. Neither ACC nor crystalline CaCO3 is observed on -CH3 surface. Our findings present a valuable model to understand the CaCO3 biomineralization pathway in natural system where functional groups composition plays a determining role during calcium carbonate crystallization.
四种自组装单分子层表面分别含有 -COOH、-OH、-NH2 和 -CH3 官能团，用于在低 Ca(2+)浓度下定向碳酸钙 (CaCO3) 的生物矿化过程，并进一步探索了在 12 小时内成核和初始结晶的机制。在 -COOH 表面上，成核主要通过离子聚集机制发生，而预成核离子簇也可能参与其中。然而，在 -OH 和 -NH2 表面上，成核通过碳酸钙簇形成，这些簇在溶液中聚集，然后在无定形碳酸钙 (ACC) 成核后被吸附到表面上。此外，带负电荷的强 -COOH 表面有利于方解石的直接形成，而 -OH 和 -NH2 表面决定了具有优先晶向的文石的形成。-CH3 表面上既没有 ACC 也没有结晶 CaCO3。我们的发现为理解自然系统中 CaCO3 生物矿化途径提供了一个有价值的模型，其中官能团组成在碳酸钙结晶过程中起着决定性的作用。
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