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I. Synthesis and Proton Conductivity Studies of Mesostructured Organosilicates and Bitriazole-Polymer Composites. II. Targeted Nanoparticles for siRNA Delivery

機(jī)譯：I.介孔結(jié)構(gòu)有機(jī)硅酸鹽和比特唑 - 聚合物復(fù)合材料的合成和質(zhì)子傳導(dǎo)性研究。 II。用于siRNa遞送的靶向納米顆粒

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The underlying theme of the research outlined in both parts of this report is centered on the ability to use synthetic design as a probe to investigate and answer fundamental mechanistic questions in an effort to improve the function of materials employed in energy and biological research. Specifically in the field of energy research, we have designed a new strategy aimed at improving the proton conductivity of organically modified silica-based polymer electrolyte membranes for use in direct methanol fuel cells. Our design involves the incorporation of the desired organic functional group into a siloxane-modified polymerizable surfactant that can be used in mesoporous silicate synthesis. This approach takes advantage of the silicate assembly mechanism, which places surfactants exclusively within the pores of the silicate at high loadings. The desired functional group is revealed upon selective cleavage after hydrothermal silicate synthesis. We have used this approach to synthesize organosilicates with different sized organic groups displaying high organic acid densities and have studied their proton conductivity under fully hydrated conditions. Under these conditions, structural diffusion via a percolated water network is the dominant mechanism of proton transport.ududWith regards to membranes for use in hydrogen fuel cells that operate best at temperatures above the dew point of water, the need for an alternative to water as the proton conducting medium is desired. Towards this end, we designed a new nitrogen-containing heterocycle (NCH), 4,4-1H-1H-bi-1,2,3-triazole (bitriazole) capable of mimicking water in the solid state and have investigated its ability to conduct protons in the presence of polyethylene oxides under anhydrous conditions. With numerous chemical tools at our disposal, we probed the mechanism of proton conduction and confirmed the bitriazole proton to be the source of anhydrous proton conductivity. Our data suggests structural diffusion as the dominant transport mechanism via synergistic interactions between bitriazole and polyethylene oxides in the polymer-rich region of the composite material that is encapsulated by a crystalline nonconductive bitriazole framework.ududIn the second part of this report, we shift our focus to the investigation of antibody-mediated targeting, using our well-established cyclodextrin polycation (CDP) nanoparticles containing therapeutic oligonuleotides, to epitopes expressed at the surface of cancer cells as a means of increasing site-specific therapeutic delivery. To do this, we synthesized fragments of anti-CD20 (rituximab) and conjugated them to flexible poly(ethylene glycol) (PEG) linkers with terminal adamantane groups that can interact with the cyclodextrins on the surface of the CDP nanoparticle via the formation of an inclusion complex. With the PEGylated antibody fragments in hand, we investigate, via a B-cell lymphoma model, the binding characteristics of the targeting ligands as well as their effect on the binding, internalization, and efficacy of the targeted CDP-nucleic acid therapeutic nanoparticles.ud
機(jī)譯：本報(bào)告兩部分概述的研究的基本主題集中在使用合成設(shè)計(jì)作為探查和回答基本機(jī)械問(wèn)題的能力上，以改善用于能源和生物學(xué)研究的材料的功能。特別是在能源研究領(lǐng)域，我們?cè)O(shè)計(jì)了一種新的策略，旨在改善用于直接甲醇燃料電池的有機(jī)改性二氧化硅基聚合物電解質(zhì)膜的質(zhì)子傳導(dǎo)性。我們的設(shè)計(jì)涉及將所需的有機(jī)官能團(tuán)摻入可用于介孔硅酸鹽合成的硅氧烷改性的可聚合表面活性劑中。這種方法利用了硅酸鹽組裝機(jī)制的優(yōu)勢(shì)，該機(jī)制將表面活性劑僅在高載荷下專(zhuān)門(mén)置于硅酸鹽的孔內(nèi)。在水熱硅酸鹽合成后，選擇性裂解顯示所需的官能團(tuán)。我們已經(jīng)使用這種方法來(lái)合成具有高有機(jī)酸密度的不同尺寸有機(jī)基團(tuán)的有機(jī)硅酸鹽，并研究了它們?cè)谕耆蠗l件下的質(zhì)子傳導(dǎo)性。在這些條件下，通過(guò)滲透水網(wǎng)絡(luò)的結(jié)構(gòu)擴(kuò)散是質(zhì)子傳輸?shù)闹饕獧C(jī)制。 ud ud關(guān)于用于氫燃料電池的膜最好在高于水露點(diǎn)的溫度下工作，因此需要一種替代方法需要水作為質(zhì)子傳導(dǎo)介質(zhì)。為此，我們?cè)O(shè)計(jì)了一種新型的能夠模擬固態(tài)水的含氮雜環(huán)（NCH）4,4-1H-1H-bi-1,2,3-三唑（bitriazole），并研究了其能夠模擬水的能力。在無(wú)水條件下在聚環(huán)氧乙烷存在下傳導(dǎo)質(zhì)子利用我們可用的多種化學(xué)工具，我們探究了質(zhì)子傳導(dǎo)的機(jī)理，并確認(rèn)了三唑質(zhì)子是無(wú)水質(zhì)子傳導(dǎo)性的來(lái)源。我們的數(shù)據(jù)表明結(jié)構(gòu)擴(kuò)散是通過(guò)在復(fù)合材料的富含聚合物的區(qū)域（由結(jié)晶的非導(dǎo)電性的三苯并氮骨架）封裝的三苯并三唑與聚環(huán)氧乙烷之間的協(xié)同相互作用作為主要的傳輸機(jī)制。 ud ud在本報(bào)告的第二部分中，我們將我們的重點(diǎn)轉(zhuǎn)移到研究抗體介導(dǎo)的靶向上，使用我們公認(rèn)的含有治療性寡核苷酸的環(huán)糊精聚陽(yáng)離子（CDP）納米粒子，將其轉(zhuǎn)移至癌細(xì)胞表面表達(dá)的表位，作為增加部位特異性治療傳遞的手段。為此，我們合成了抗CD20（rituximab）片段并將其綴合到具有末端金剛烷基團(tuán)的柔性聚乙二醇（PEG）接頭上，該末端可與CDP納米顆粒表面上的環(huán)糊精相互作用，形成環(huán)糊精。包容性。有了PEG化的抗體片段，我們將通過(guò)B細(xì)胞淋巴瘤模型研究靶向配體的結(jié)合特征，以及它們對(duì)靶向CDP核酸治療性納米粒子的結(jié)合，內(nèi)在化和功效的影響。 ud

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    Alabi Akinleye Christopher;

  • 作者單位
  • 年度 2009
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