Collaborative Research: Characterization and Optimization of N-Heterocyclic Carbene Functionalized Nanoparticle Systems

合作研究：N-杂环卡宾功能化纳米颗粒系统的表征和优化

• 批准号: 2108328
• 负责人: David Jenkins
• 金额: $ 36.59万
• 依托单位: University of Tennessee Knoxville
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-07-01 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2108328&HistoricalAwards=false
• 关键词: Collaborative; Research; Characterization; Optimization; Heterocyclic

With the support of the Macromolecular, Supramolecular, and Nanochemistry Program in the Division of Chemistry, Dr. David Jenkins of the University of Tennessee and Drs. Jon Camden and Gina Navoa Svarovsky of the University of Notre Dame explore the use of N-heterocyclic carbenes (NHCs) chemistry for the surface modification of gold nanoparticles. Gold nanoparticles, which are typically stabilized by charged molecules such as citrate or monolayers with thiol anchoring groups, are used in wide-ranging chemical, biological, and environmental technologies but use is limited by the inherent instability of the nanoparticles in water. Drs. Jenkins and Camden are identifying ways to overcome this limitation by using NHC ligands. To do so, they are using a top-down method that involves the initial coordination of these ligands to coinage metal ions before being transferred to gold nanoparticle surfaces. They are using a variety of characterization tools to evaluate this chemistry and to better understand what NHC ligands promote enhanced stability of the functionalized gold nanoparticles. Drs. Jenkins, Camden, and Svarovsky are pursuing a Teaching Fellows Residency program to create an immersive research experience in the research laboratories and a Student Engagement in Authentic Science (SEAS) program that engages middle school students with original scientific data.The research involves the synthesis, characterization, and transfer of metal NHC complexes to gold nanoparticle surfaces, the characterization of the resulting bonding and close packing of a library of NHC ligands on gold nanoparticles, and the subsequent evaluation of NHC-functionalized gold stability and longevity. All of these studies utilize a top-down approach wherein the gold nanoparticles are functionalized after isolated coinage metal NHC complexes have formed in solution. This universal, top-down strategy is expected to be broadly applicable to gold nanoparticles of varying shapes and sizes. This approach has the potential to overcome limitations associated with bottom-up functionalization steps where each individual reaction is typically optimized for a specific system. Gold nanoparticles functionalized with heterocyclic carbenes hold promise in the quest to overcome challenges faced by conventional surface chemistries.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系大分子、超分子和纳米化学项目的支持下，田纳西大学的大卫詹金斯博士和圣母大学的乔恩·卡姆登博士和吉娜·纳沃亚·斯瓦罗夫斯基博士探索使用N-杂环卡宾（NHC）化学对金纳米颗粒进行表面改性。金纳米颗粒通常由带电分子如柠檬酸盐或具有硫醇锚定基团的单层稳定，用于广泛的化学，生物和环境技术，但使用受到纳米颗粒在水中固有的不稳定性的限制。Jenkins和Camden博士正在通过使用NHC配体来确定克服这种限制的方法。为此，他们使用了一种自上而下的方法，该方法涉及这些配体在转移到金纳米颗粒表面之前与钴金属离子的初始配位。他们正在使用各种表征工具来评估这种化学性质，并更好地了解NHC配体促进功能化金纳米粒子的稳定性增强。Jenkins博士、Camden博士和Svarovsky博士正在进行一项教学研究员驻留计划，以在研究实验室中创造沉浸式研究体验，以及一项学生参与真实科学（SEAS）计划，该计划让中学生参与原始科学数据。该研究涉及金属NHC络合物的合成、表征和转移到金纳米颗粒表面，表征所得到的NHC配体库在金纳米颗粒上的键合和紧密堆积，以及随后评估NHC官能化金的稳定性和寿命。所有这些研究都利用自上而下的方法，其中在溶液中形成分离的钴金属NHC络合物之后，将金纳米颗粒官能化。这种普遍的、自上而下的策略有望广泛适用于不同形状和大小的金纳米颗粒。这种方法有可能克服与自下而上的官能化步骤相关的限制，其中每个单独的反应通常针对特定系统进行优化。用杂环卡宾功能化的金纳米颗粒有望克服传统表面化学所面临的挑战。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Ad aurum: tunable transfer of N-heterocyclic carbene complexes to gold surfaces

• DOI: 10.1039/d2qi01941h
• 发表时间: 2022-10-17
• 期刊: INORGANIC CHEMISTRY FRONTIERS
• 影响因子: 7
• 作者: Dominique, Nathaniel L.;Chen, Ran;Camden, Jon P.
• 通讯作者: Camden, Jon P.

Giving Gold Wings: Ultrabright and Fragmentation Free Mass Spectrometry Reporters for Barcoding, Bioconjugation Monitoring, and Data Storage

赋予金翼：用于条形码、生物共轭监测和数据存储的超亮、无碎片质谱报告仪

• DOI: 10.1002/anie.202219182
• 发表时间: 2023
• 期刊: Angewandte Chemie International Edition
• 作者: Dominique, Nathaniel L.;Jensen, Isabel M.;Kaur, Gurkiran;Kotseos, Chandler Q.;Boggess, William C.;Jenkins, David M.;Camden, Jon P.
• 通讯作者: Camden, Jon P.

Probing N-Heterocyclic Carbene Surfaces with Laser Desorption Ionization Mass Spectrometry

用激光解吸电离质谱法探测 N-杂环卡宾表面

• DOI: 10.1021/acs.analchem.1c02401
• 发表时间: 2021
• 期刊: Analytical Chemistry
• 影响因子: 7.4
• 作者: Dominique, Nathaniel L.;Strausser, Shelby L.;Olson, Jacob E.;Boggess, William C.;Jenkins, David M.;Camden, Jon P.
• 通讯作者: Camden, Jon P.