期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 40, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202208475
关键词
Antiscalants; Crystal Engineering; Green Chemistry; Reaction Mechanisms; Solid-State REDOR NMR
资金
- Procter Gamble Inc.
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [251939425]
- Israel Science Foundation grant [2001/17]
- Projekt DEAL
This study reveals the molecular mechanisms by which small-molecular-weight additives impact amorphous calcium carbonate (ACC), stabilizing its structure and preventing crystallization through interactions with prenucleation clusters (PNCs). These findings are significant for understanding the role of small-MW molecules in crystallization and biomineralization, and provide a theoretical basis for the development of new sustainable antiscalants.
Small-molecular-weight (MW) additives can strongly impact amorphous calcium carbonate (ACC), playing an elusive role in biogenic, geologic, and industrial calcification. Here, we present molecular mechanisms by which these additives regulate stability and composition of both CaCO3 solutions and solid ACC. Potent antiscalants inhibit ACC precipitation by interacting with prenucleation clusters (PNCs); they specifically trigger and integrate into PNCs or feed PNC growth actively. Only PNC-interacting additives are traceable in ACC, considerably stabilizing it against crystallization. The selective incorporation of potent additives in PNCs is a reliable chemical label that provides conclusive chemical evidence that ACC is a molecular PNC-derived precipitate. Our results reveal additive-cluster interactions beyond established mechanistic conceptions. They reassess the role of small-MW molecules in crystallization and biomineralization while breaking grounds for new sustainable antiscalants.
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