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Regulating Nucleation Kinetics through Molecular Interactions at the Polymer-Solute Interface

机译：通过聚合物-溶质界面上的分子相互作用调节成核动力学。

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摘要

Heterogeneous nucleation is ubiquitous both in nature and in industrial practice; therefore, the ability to inhibit or enhance the kinetics of a crystallization process is essential in many scientific and technological areas. In order to better understand the role of surface functionality in regulating the nucleation rate, six commercially available polymers have been used as heteronucleants of acetaminophen (ACM) molecules: polydimethylsiloxane (PDMS) with siloxane functional groups Si-O-Si forming the backbone of silicones, partially fluorinated elastomer polyvinylidenedifluoride (PVDF), polystyrene (PS) having weak electron-donor phenyl rings, poly(n-buthyl methacrylate) (PnBMA) showing ester functionality, polyimide (PI) that includes both hydrogen-bond acceptor imide functionality and carbonyl groups, ethylene/acrylic acid (EAA) copolymer with carboxyl moiety. Experimental results from induction time statistics, van Oss-Chaudhury-Good model of surface energetics, and powder X-ray diffraction (PXRD) analysis showed that polymeric interfaces promoting specific acid-base interactions and directionally ordered reorganization of molecules led to enhanced nucleation kinetics, while the formation of nuclei was retarded on hydrophobic films that did not induce preferential orientations of the crystalline facets.
机译：自然界和工业实践中都普遍存在异相形核。因此，在许多科学技术领域，抑制或增强结晶过程动力学的能力至关重要。为了更好地了解表面官能度在调节成核速率中的作用，已使用六种市售聚合物作为对乙酰氨基酚（ACM）分子的杂成核剂：具有硅氧烷官能团Si-O-Si的聚二甲基硅氧烷（PDMS），形成硅氧烷的主链，部分氟化的弹性体聚偏二氟乙烯（PVDF），具有弱电子给体苯环的聚苯乙烯（PS），具有酯官能度的聚甲基丙烯酸正丁酯（PnBMA），同时包含氢键受体酰亚胺官能团和羰基的聚酰亚胺（PI）基团，具有羧基部分的乙烯/丙烯酸（EAA）共聚物。感应时间统计，表面能学的van Oss-Chaudhury-Good模型和粉末X射线衍射（PXRD）分析的实验结果表明，聚合物界面促进了特定的酸碱相互作用和分子的定向有序重组，从而提高了成核动力学，而在不诱导结晶面优先取向的疏水膜上，核的形成被延迟了。

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