纳米限域下不饱和钙溶液中的粘弹性界面结构

中文摘要 AI 辅助

钙矿化是从生物矿化到规模化碳封存等过程的基础，但成核的最早阶段仍未得到解决。本研究在体相碳酸钙沉淀仍处于不饱和状态的条件下，探究了纳米限域环境下的含钙溶液。通过灵敏的表面力测量，我们识别出一种为钙溶液所特有的长程非DLVO排斥相互作用，将其归因于矿物界面处的水合离子网络。这些界面网络表现出与体相溶液不同的粘弹性行为，在宽pH范围内持续存在，且可被具有强表面亲和力的竞争离子破坏。我们的发现提供了实验证据，表明在不饱和条件下，矿物界面处可形成稳定的水合离子网络，支持界面与限域可稳定成核前的中间离子聚集体的可能性。这些结果弥合了矿物成核的经典与非经典描述，并强调了界面与限域在调控结晶路径中的核心作用。

英文摘要

Calcium mineralisation underpins processes ranging from biomineralisation to scalable carbon storage, yet the earliest stages of nucleation remain unresolved. Here we investigate calcium-containing solutions under nanoscopic confinement while remaining undersaturated with respect to bulk calcium carbonate precipitation. Using sensitive surface force measurements, we identify a long-range non-DLVO repulsive interaction specific to calcium solutions, which we attribute to hydrated ion networks at mineral interfaces. These interfacial networks exhibit viscoelastic behaviour distinct from the bulk solution, persist across a broad pH range, and can be disrupted by competing ions with strong surface affinity. Our findings provide experimental evidence that stable hydrated ion networks can emerge at mineral interfaces under undersaturated conditions, supporting the possibility that interfaces and confinement stabilise intermediate ion assemblies prior to nucleation. These results bridge classical and nonclassical descriptions of mineral nucleation and highlight the central role of interfaces and confinement in directing crystallisation pathways.

发表机构

• Department of Chemistry, Physical & Theoretical Chemistry Laboratory, University of Oxford（牛津大学化学系物理与理论化学实验室）

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