Ultralow protein adsorbing coatings from clickable PEG nanogel solutions: benefits of attachment under salt-induced phase separation conditions and comparison with PEG/albumin nanogel coatings.
Ultralow protein adsorbing coatings from clickable PEG nanogel solutions: benefits of attachment under salt-induced phase separation conditions and comparison with PEG/albumin nanogel coatings.
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DOI：
10.1021/la3051115
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发表时间：
2013-03-26
期刊：
影响因子：
--
通讯作者：
Elbert DL
中科院分区：
文献类型：
--
作者：
Donahoe CD;Cohen TL;Li W;Nguyen PK;Fortner JD;Mitra RD;Elbert DL
通过使用铜催化的叠氮化物/炔环加成（CuAAC）到叠氮化物和炔官能化的聚（乙二醇）（PEG）单体的部分水溶液中来合成可点击的纳米凝胶溶液。使用第二点击反应制造涂层：纳米凝胶溶液与巯基硅烷化玻璃的UV硫醇-炔附着。由于通过添加铜螯合剂有效地停止了CuAAC反应，因此我们能够在不存在溶液反应的情况下防止本体凝胶化并将涂层厚度限制为纳米凝胶的单个单层。这使得能够包含亲液盐，这导致PEG相分离并使纳米凝胶堆积密度几乎加倍，如通过具有耗散的石英晶体微天平（QCM-D）所证实的。通过全内反射荧光（TIRF）显微镜和细胞粘附测定的单分子计数分析蛋白吸附。由附接有盐的相分离的可点击纳米凝胶溶液形成的涂层比测试的其他100%PEG涂层以及聚-L-赖氨酸-g-PEG（PLL-g-PEG）涂层吸附显著更少的纤维蛋白原。然而，PEG/白蛋白纳米凝胶涂层仍然优于最好的100%PEG可点击纳米凝胶涂层。可点击纳米凝胶涂层在铜存在下的额外表面交联进一步降低了纤维蛋白原吸附水平，更接近于PEG/白蛋白纳米凝胶涂层的水平。然而，这一步骤对细胞粘附的长期抗性产生了负面影响，并通过原子力显微镜（AFM）显着改变了涂层的形态。点击策略的主要益处是部分聚合的溶液几乎无限期地稳定，允许在相分离状态下附着而没有本体凝胶化的危险，从而产生我们迄今为止研究的性能最好的100%PEG涂层。
Clickable nanogel solutions were synthesized by using the copper catalyzed azide/alkyne cycloaddition (CuAAC) to partially polymerize solutions of azide and alkyne functionalized poly(ethylene glycol) (PEG) monomers. Coatings were fabricated using a second click reaction: a UV thiol-yne attachment of the nanogel solutions to mercaptosilanated glass. Because the CuAAC reaction was effectively halted by the addition of a copper-chelator, we were able to prevent bulk gelation and limit the coating thickness to a single monolayer of nanogels in the absence of the solution reaction. This enabled the inclusion of kosmotropic salts, which caused the PEG to phase-separate and nearly double the nanogel packing density, as confirmed by Quartz Crystal Microbalance with Dissipation (QCM-D). Protein adsorption was analyzed by single molecule counting with total internal reflection fluorescence (TIRF) microscopy and cell adhesion assays. Coatings formed from the phase-separated clickable nanogel solutions attached with salt adsorbed significantly less fibrinogen than other 100% PEG coatings tested, as well as poly-L-lysine-g-PEG (PLL-g-PEG) coatings. However, PEG/albumin nanogel coatings still outperformed the best 100% PEG clickable nanogel coatings. Additional surface crosslinking of the clickable nanogel coating in the presence of copper further reduced levels of fibrinogen adsorption closer to those of PEG/albumin nanogel coatings. However, this step negatively impacted long-term resistance to cell adhesion and dramatically altered the morphology of the coating by atomic force microscopy (AFM). The main benefit of the click strategy is that the partially polymerized solutions are stable almost indefinitely, allowing attachment in the phase-separated state without danger of bulk gelation, and thus, producing the best performing 100% PEG coating that we have studied to date.
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DOI：
10.1021/la804077t
发表时间：
2009-05-19
期刊：
Langmuir : the ACS journal of surfaces and colloids
影响因子：
--
作者：
Hudalla GA;Murphy WL
通讯作者：
Murphy WL
影响因子：
2.1
作者：
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影响因子：
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作者：
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影响因子：
14
作者：
Kizilel, S;Sawardecker, E;Pérez-Luna, VH
通讯作者：
Pérez-Luna, VH
影响因子：
4.9
作者：
Bridges, Amanda W.;Whitmire, Rachel E.;Garcia, Andres J.
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