Stable Organic Interfaces Having Unnatural Compositions: Nanoscale Control of Heterogeneity

具有非自然成分的稳定有机界面：异质性的纳米级控制

• 批准号: 1710561
• 负责人: T. Randall Lee
• 金额: $ 45万
• 依托单位: University of Houston
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-11-01 至 2021-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1710561&HistoricalAwards=false
• 关键词: Stable; Organic; Interfaces; Having; Unnatural

Professor T. Randall Lee of the University of Houston is supported by the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry to design and synthesize new organic chemical agents. A major goal of the proposed research is to tune the chemical composition of thin organic coatings to afford surfaces with compositions that are not found in nature. Given the unique compositions targeted, the coatings are likely to be extraordinarily non-adhesive and therefore useful for coating not only electronic devices (e.g., ultrathin cell phones, laptops, and flat-screen televisions), but also artificial implants (e.g., heart stents) and nanoparticles for medical applications (e.g., cancer therapy). During the grant period, the PI seeks to broaden the participation of women and minorities through several educational/outreach activities, including the Welch Summer Scholars program, the UH STEM Center, the NSF-supported Houston Louis Stokes Alliance for Minority Participation (H-LSAMP) program, and visits to campus and research mentoring for local high school students. The proposed research seeks to design, synthesize, and utilize multidentate adsorbates for the generation of unnatural "conflicted" self-assembled monolayers (SAMs) on gold. Three systems of current technological interest are emphasized: (1) the design and synthesis of multidentate adsorbates for fabricating highly stable thin-film coatings with uniquely controlled surface composition of chemical entities that are either phase incompatible or structurally dissimilar, for the purpose of generating homogeneously mixed heterogeneous "conflicted" interfaces; (2) the use of specifically fluorinated adsorbate molecules to generate nanoscale films having well-defined composition and structure, with an ultimate goal of defining the critical elements (e.g., minimum degree of fluorination) needed to construct organic interfaces with controlled hydrophobicity, anti-adhesiveness, and lubricity; and (3) the generation and study of thin-film architectures, including surface-grafted oligomeric films, in which the terminal functional groups mimic the backbones of industrially relevant polymers, with the goal of evaluating the interfacial properties and reactivity of well-defined polymer surfaces. Advantages offered by the targeted multidentate adsorbates include films with markedly greater stability than those derived from n-alkanethiols, leading in part to advances in nanoscale lubrication, corrosion resistance, nanoparticle stabilization, and anti-adhesive coatings. Furthermore, due to the restricted surface mobility of the multidentate adsorbates, mixed monolayers of these adsorbates functionalized with disparate chemical tailgroups offer "conflicted" organic nanoscale coatings with tailored chemical heterogeneity and controlled nanoscale roughness.

T教授休斯顿大学的Randall Lee得到化学系大分子，超分子和纳米化学项目的支持，设计和合成新的有机化学试剂。 拟议研究的一个主要目标是调整薄有机涂层的化学成分，以提供具有自然界中没有的成分的表面。 考虑到目标的独特组合物，涂层可能是非常非粘性的，因此不仅可用于涂覆电子器件（例如，手机、笔记本电脑和平板电视），而且还有人工植入物（例如，心脏支架）和用于医疗应用的纳米颗粒（例如，癌症治疗）。 在赠款期间，PI旨在通过几个教育/外联活动，包括韦尔奇夏季学者计划，UH STEM中心，NSF支持的休斯顿路易斯斯托克斯少数民族参与联盟（H-LSAMP）计划，以及访问校园和研究指导当地高中学生扩大妇女和少数民族的参与。 拟议的研究旨在设计，合成，并利用多齿吸附剂的非自然的“冲突”的自组装单分子膜（SAMs）的黄金。 重点介绍了三种目前具有重要技术意义的体系：（1）设计和合成多齿吸附剂，用于制备具有独特控制的表面化学成分的高稳定薄膜涂层，这些化学成分要么是相不相容的，要么是结构上不同的，目的是产生均匀混合的异质“冲突”界面;（2）使用特定氟化的吸附物分子来产生具有明确定义的组成和结构的纳米级膜，最终目标是定义关键元素（例如，最小程度的疏水性）;和（3）薄膜结构的产生和研究，包括表面接枝的低聚物膜，其中末端官能团模拟工业相关聚合物的主链，目的是评估界面性质和明确定义的聚合物表面的反应性。 由目标多齿吸附物提供的优点包括具有比源自正烷硫醇的那些膜显著更大的稳定性的膜，部分导致纳米级润滑、耐腐蚀性、纳米颗粒稳定化和防粘涂层的进步。 此外，由于多齿吸附物的受限表面流动性，用不同的化学尾基官能化的这些吸附物的混合单层提供具有定制的化学异质性和受控的纳米级粗糙度的“冲突”有机纳米级涂层。

项目成果

Quaternary Ammonium-Terminated Films Formed from Mixed Bidentate Adsorbates Provide a High-Capacity Platform for Oligonucleotide Delivery

由混合双齿吸附物形成的季铵封端薄膜为寡核苷酸递送提供高容量平台

• DOI: 10.1021/acsami.8b12244
• 发表时间: 2018
• 期刊: ACS Applied Materials & Interfaces
• 影响因子: 9.5
• 作者: Hoang, Johnson;Park, Chul Soon;Lee, Han Ju;Marquez, Maria D.;Zenasni, Oussama;Gunaratne, Preethi H.;Lee, T. Randall
• 通讯作者: Lee, T. Randall

Hydrophilic surfaces via the self-assembly of nitrile-terminated alkanethiols on gold

通过金上末端腈链烷硫醇的自组装形成亲水表面

• DOI: 10.3934/matersci.2018.2.171
• 发表时间: 2018
• 期刊: AIMS Materials Science
• 影响因子: 1.8
• 作者: Soon Park, Chul;Zenasni, Oussama;D. Marquez, Maria;Justin Moore, H.;Randall Lee, T.
• 通讯作者: Randall Lee, T.

Contrasting Transport and Electrostatic Properties of Selectively Fluorinated Alkanethiol Monolayers with Embedded Dipoles

• DOI: 10.1021/acs.jpcc.7b11892
• 发表时间: 2018-03-08
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY C
• 影响因子: 3.7
• 作者: Bruce, Robert C.;You, Lin;Hacker, Christina A.
• 通讯作者: Hacker, Christina A.

Mimicking Polymer Surfaces Using Cyclohexyl- and Perfluorocyclohexyl-Terminated Self-Assembled Monolayers

使用环己基和全氟环己基封端的自组装单层模拟聚合物表面

• DOI: 10.1021/acsanm.9b01268
• 发表时间: 2019
• 期刊: ACS Applied Nano Materials
• 影响因子: 5.9
• 作者: Yu, Tianlang;Marquez, Maria D.;Zenasni, Oussama;Lee, T. Randall
• 通讯作者: Lee, T. Randall

Full Spectrum Solar Thermal Energy Harvesting and Storage by a Molecular and Phase-Change Hybrid Material

• DOI: 10.1016/j.joule.2019.11.001
• 发表时间: 2019-12-18
• 期刊: JOULE
• 影响因子: 39.8
• 作者: Kashyap, Varun;Sakunkaewkasem, Siwakorn;Ghasemi, Hadi
• 通讯作者: Ghasemi, Hadi