The Valence-Dependent Activity of Colloidal Molecules as Ice Recrystallization Inhibitors,ACS Macro Letters

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The Valence-Dependent Activity of Colloidal Molecules as Ice Recrystallization Inhibitors
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-07-15 , DOI: 10.1021/acsmacrolett.4c00331
Xiaoqian Tian ₁ , Huangbing Xu _{1,

2} , Teng Qiu _{1,

2} , Fengjiao Wu ₂ , Xiaoyu Li _{1,

2} , Longhai Guo _{1,

2}

Affiliation

Inspired by advances in cryopreservation techniques, which are essential for modern biomedical applications, there is a special interest in the ice recrystallization inhibition (IRI) of the antifreeze protein (AFPs) mimics. There are in-depth studies on synthetic materials mimicking AFPs, from simple molecular structure levels to complex self-assemblies. Herein, we report the valence-dependent IRI activity of colloidal organic molecules (CMs). The CMs were prepared through polymerization-induced particle-assembly (PIPA) of the ABC-type triblock terpolymer of poly(acryloxyethyl trimethylammonium chloride)-b-poly(benzyl acrylate)-b-poly(diacetone acrylamide) (PATAC-b-PBzA-b-PDAAM) at high monomer conversions. Stabilized by the cationic block of PATAC, the strong intermolecular H-bonding and incompatibility of the PDAAM block with PBzA contributed to the in situ formation of Janus particles (AX₁) beyond the initial spherical seed particles (AX₀), as well as the high valency clusters of linear AX₂ and trigonal AX₃. Their distribution was controlled mainly by the polymerization degrees (DPs) of PATAC and PDAAM blocks. IRI activity results of the CMs suggest that the higher fraction of AX₁ results in the better IRI activity. Increasing the fraction of AX₁ from 27% to 65% led to a decrease of the mean grain size from 39.8% to 10.9% and a depressed growth rate of ice crystals by 58%. Moreover, by replacing the PDAAM block with the temperature-responsive one of poly(N-isopropylacrylamide) (PNIPAM), temperature-adjustable IRI activity was observed, which is well related to the reversible transition of AX₀ to AX₁, providing a new idea for the molecular design of amphiphilic polymer nanoparticle-based IRI activity materials.

中文翻译：

胶体分子作为冰再结晶抑制剂的价态依赖性活性

受冷冻保存技术进步的启发（这对现代生物医学应用至关重要），人们对抗冻蛋白（AFP）模拟物的冰重结晶抑制（IRI）特别感兴趣。人们对模仿 AFP 的合成材料进行了深入的研究，从简单的分子结构水平到复杂的自组装。在此，我们报告了胶体有机分子（CM）的价态依赖性 IRI 活性。 CM是通过聚(丙烯酰氧基乙基三甲基氯化铵) -b-聚(丙烯酸苄酯) -b-聚(双丙酮丙烯酰胺)(PATAC -b -PBzA)的ABC型三嵌段三元共聚物的聚合诱导颗粒组装(PIPA)制备的- b -PDAAM) 在高单体转化率下。通过 PATAC 的阳离子嵌段稳定，PDAAM 嵌段与 PBzA 之间的强分子间氢键和不相容性有助于在初始球形种子颗粒 (AX ₀ ) 之外原位形成 Janus 颗粒 (AX ₁ )，以及线性 AX ₂和三角 AX ₃的高价簇。它们的分布主要由 PATAC 和 PDAAM 嵌段的聚合度 (DP) 控制。 CM 的 IRI 活性结果表明 AX ₁的比例越高，IRI 活性越好。将 AX ₁的比例从 27% 增加到 65% 导致平均晶粒尺寸从 39.8% 减小到 10.9%，冰晶生长速率降低 58%。此外，通过用温度响应型聚（ N-异丙基丙烯酰胺）（PNIPAM）取代PDAAM嵌段，观察到温度可调的IRI活性，这与AX ₀到AX ₁的可逆转变密切相关，提供了一种新的方法。基于两亲性聚合物纳米颗粒的 IRI 活性材料的分子设计理念。

更新日期：2024-07-15

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