Two-Dimensional Triblock Peptide Assemblies for the Stabilization of Pickering Emulsions with pH Responsiveness.
Two-Dimensional Triblock Peptide Assemblies for the Stabilization of Pickering Emulsions with pH Responsiveness.
复制标题
DOI：
10.1021/acsami.2c17558
复制
发表时间：
2022-11-30
影响因子：
9.5
通讯作者：
Keddie, Joseph L.
中科院分区：
文献类型：
--
作者：
Huang, Zhiwei;Calicchia, Eleonora;Jurewicz, Izabela;Munoz, Edgar;Garriga, Rosa;Portale, Giuseppe;Howlin, Brendan J.;Keddie, Joseph L.
关键词：
已知多种二维（2D）纳米材料，包括氧化石墨烯和粘土，可以稳定皮克林乳液，以制造用于传感器、催化剂和封装功能的结构。本文介绍了一种以自组装的两亲性三嵌段寡聚甘氨酸为乳化剂的新型Pickering乳液。肽两亲物对环境变化更敏感（例如，pH、温度和离子强度）比无机2D材料更好，无机2D材料具有化学刚性的面内结构。肽分子之间的非共价力随环境而变化，从而赋予响应性。我们提供了新的证据，双触角寡甘氨酸，Gly 4-NH-C10 H20-NH-Gly 4，自组装成二维血小板结构，表示为tectomers，在溶液中，在中性缓冲pH值使用小角X射线散射和分子动力学模拟。分子以线性构象而不是U形堆叠在片晶中。我们发现，层状低聚甘氨酸血小板吸附在油/水界面和稳定的水包油乳液。这是首次报道将2D寡聚甘氨酸血小板用作皮克林稳定剂。该乳液在酸性环境中显示出强烈的pH响应。因此，在降低pH值时，寡聚甘氨酸的末端氨基的质子化由于排斥静电力而引起层状结构的解体，从而导致乳液不稳定。为了证明该材料的应用，我们表明，模型的活性成分，β-胡萝卜素，在油中的pH值降低时释放。有趣的是，在pH 9缓冲液中，随着时间的推移，油滴的形态演变，作为寡聚甘氨酸稳定剂逐步创建一个较厚的界面层。该演示开辟了一条新的路线，使用自组装合成肽两亲物来稳定Pickering乳液，这对于生物医学和制药应用具有重要意义。
A variety of two-dimensional (2D) nanomaterials, including graphene oxide and clays, are known to stabilize Pickering emulsions to fabricate structures for functions in sensors, catalysts, and encapsulation. We introduce here a novel Pickering emulsion using self-assembled amphiphilic triblock oligoglycine as the emulsifier. Peptide amphiphiles are more responsive to environmental changes (e.g., pH, temperature, and ionic strength) than inorganic 2D materials, which have a chemically rigid, in-plane structure. Noncovalent forces between the peptide molecules change with the environment, thereby imparting responsiveness. We provide new evidence that the biantennary oligoglycine, Gly4–NH–C10H20–NH–Gly4, self-assembles into 2D platelet structures, denoted as tectomers, in solution at a neutral buffered pH using small-angle X-ray scattering and molecular dynamics simulations. The molecules are stacked in the platelets with a linear conformation, rather than in a U-shape. We discovered that the lamellar oligoglycine platelets adsorbed at an oil/water interface and stabilized oil-in-water emulsions. This is the first report of 2D oligoglycine platelets being used as a Pickering stabilizer. The emulsions showed a strong pH response in an acidic environment. Thus, upon reducing the pH, the protonation of the terminal amino groups of the oligoglycine induced disassembly of the lamellar structure due to repulsive electrostatic forces, leading to emulsion destabilization. To demonstrate the application of the material, we show that a model active ingredient, β-carotene, in the oil is released upon decreasing the pH. Interestingly, in pH 9 buffer, the morphology of the oil droplets evolved over time, as the oligoglycine stabilizer created progressively a thicker interfacial layer. This demonstration opens a new route to use self-assembled synthetic peptide amphiphiles to stabilize Pickering emulsions, which can be significant for biomedical and pharmaceutical applications.
登录
查看更多内容
DOI：
10.1039/d1tc02753k
发表时间：
2021-11-25
期刊：
Journal of materials chemistry. C
影响因子：
--
作者：
Dong J;Sami S;Balazs DM;Alessandri R;Jahani F;Qiu L;Marrink SJ;Havenith RWA;Hummelen JC;Loi MA;Portale G
通讯作者：
Portale G
影响因子：
21.8
作者：
Frederix, Pim W. J. M.;Scott, Gary G.;Tuttle, Tell
通讯作者：
Tuttle, Tell
影响因子：
0.8
作者：
Bovin, N. V.;Tuzikov, A. B.;Chinarev, A. A.
通讯作者：
Chinarev, A. A.
影响因子：
3.4
作者：
Cook, Alexander B.;Schlich, Michele;Palange, Anna Lisa
通讯作者：
Palange, Anna Lisa
影响因子：
8.8
作者：
Cui, Leqi;Cho, Hyung Taek;Park, Yeonhwa
通讯作者：
Park, Yeonhwa