Metalloenzyme Mimics with Unsupported Metal Nanoparticle Catalysts

无载体金属纳米颗粒催化剂的金属酶模拟物

基本信息

批准号：
9074496
负责人：
Young Shon
金额：
$ 11.05万
依托单位：
CALIFORNIA STATE UNIVERSITY LONG BEACH
依托单位国家：
美国
项目类别：
财政年份：
2011
资助国家：
美国
起止时间：
2011-07-01 至 2020-04-30
项目状态：
已结题

来源：
https://reporter.nih.gov/project-details/9074496
关键词：
Academic support Adsorption Affect Alkenes Alkynes Amino Acids Area Attention Basic Science Behavior Binding Biochemical Biological Biological Models Biological Phenomena Biotechnology CCL7 gene Caliber Catalysis Characteristics Chemicals Chemistry Complex Constitutional Covalent Interaction Data Data Analyses Data Set Development Diffusion Enrollment Environment Enzymes Equilibrium Evaluation Exhibits Familiarity Female Funding Goals Hispanic-serving Institution Hydrocarbons Hydrogenation Information Dissemination Interdisciplinary Study Investigation Isomerism Knowledge Laboratory Research Learning Ligands Literature Medical Research Metals Methods Minority Access Minority Participation Modeling Molecular Conformation Nanotechnology Optics Palladium Participant Pattern Performance Property Publishing Reaction Recruitment Activity Reporting Research Research Activity Research Infrastructure Research Methodology Research Personnel Role Scientist Shapes Side Solubility Solvents Structure Structure-Activity Relationship Students Surface Surface Properties System Tail Techniques Technology Translational Research Travel Underrepresented Groups United States National Institutes of Health Water Work alkyl group base bridge to the baccalaureate career catalyst density design education research enzyme model experience functional group fundamental research globular protein interest learning outcome meetings metalloenzyme minority student minority undergraduate nanomaterials nanoparticle nanoparticulate nanostructured novel organic base particle programs public health relevance research study skills undergraduate research undergraduate student

项目摘要

DESCRIPTION (provided by applicant): The homogeneous catalysis based on the principle of diffusion of ligand-capped metal nanoparticles has recently drawn more interest as regards to its potential as enzyme mimics, which are one of the highest priority areas in the field of biotechnology and medical research. In particular, the ability of simple model nanostructured materials in enhancing or resisting the adsorption of particular substrates similar to that of enzymes is in needs of active investigation. Our research group has recently developed a new catalytic system that exhibits excellent activity and selectivity for the isomerization and/or hydrogenation of alkenes and alkynes. Considering their size (6-8 nm in overall particle diameter), spherical shape, and versatile ligand characteristics, the availability of these well-designed organic ligand-capped nanoparticles with active catalytic metal core will especially benefit the advancement in nanoparticle-based metalloenzyme mimics. For example, by introducing different hydrophobic functional groups in the "tail" of hydrocarbon chains of organic ligands, we can adjust steric and/or non-covalent interactions in the near-surface environment in a manner analogous to changing amino acid residues (side groups) in an enzyme binding pocket. This approach will allow the investigation of the ability of surface immobilized ligands on precisely tuning catalytic selectivity through these molecular interactions. The proposed four-year SCORE SC3 research program will focus on understanding how near-surface steric controls, non-covalent interactions, and chiral interactions determine the catalytic properties of the modified nanoparticles towards the model organic reactions relevant to the biologically important transformations (olefin reduction and isomerization). Requested funding provides summer and academic support for the PI, support for 1 post-baccalaureate fellow or technician/year, chemicals, supplies, lab consumables for research activity, and travel expenses for dissemination. The work involves four major tasks: 1) Metalloenzyme mimics with near-surface steric controls for chemo selective and regioselective reactions. 2) Metalloenzyme mimics with non-covalent interactions for chemo selective and regioselective reactions. 3) Metalloenzyme mimics with chiral interactions for stereo selective reactions. 4) Metalloenzyme mimics with controlled surface ligand polarity for biologically important reactions in water. This research plan will allow the PI to develop the basic and translational research skills to become an independent expert in nanomaterials structure controls, materials characterizations, and metalloenzyme mimics for biologically important transformations. Simultaneously, this program will provide graduate (M.S.-level, 2 students/year) and undergraduate students (4 students/year) with unique and exciting research opportunities in nanotechnology. Through enrollment in existing research-based classes, students will be offered the opportunity to be participants in an interdisciplinary research program that will collaborate on all aspects of this project - from inception, starting with basic nanoparticulate material synthesis, to completion, with the ultimate evaluation of the catalytic performance of these new metalloenzyme mimics. They will also develop the intellectual capacity to critically analyze existing information as well as develop proficiency in the analysis, interpretation and presentation of complex data sets. PI will actively recruit females and/or minority students, traditionally underrepresented groups in chemistry, to enhance the balanced advancement of research and education (CSULB is designated as a Hispanic Serving Institution). PI has a good track record of participating minority undergraduate research programs such as BUILD (Building Infrastructure Leading to Diversity funed by NIH), MARC (Minority Access to Research Careers funded by NIH), RISE (Research Initiative for Scientific Enhancement funded by NIH), BRIDGES (Bridges to the Baccalaureate funded by NIH), in addition to LSAMP (Louis Stokes Alliance for Minority Participation program funded by NSF) that are currently available in CSULB.

描述（由申请人提供）：基于配体封端的金属纳米颗粒扩散原理的均相催化最近因其作为酶模拟物的潜力而引起了更多兴趣，这是生物技术和生物技术领域最优先的领域之一。特别是，简单模型纳米结构材料增强或抵抗类似于酶的特定底物的吸附的能力需要积极研究，我们的研究小组最近开发了一种新的催化材料。该系统对烯烃和炔烃的异构化和/或氢化表现出优异的活性和选择性，考虑到它们的尺寸（总粒径为 6-8 nm）、球形和多功能配体特征，这些精心设计的有机配体的可用性。具有活性催化金属核的封端纳米颗粒将特别有利于基于纳米颗粒的金属酶模拟物的进步，例如，通过在有机烃链的“尾部”引入不同的疏水官能团。配体，我们可以以类似于改变酶结合口袋中的氨基酸残基（侧基）的方式调整近表面环境中的空间和/或非共价相互作用，这种方法将允许研究表面固定化的能力。配体在通过这些分子相互作用精确调节催化选择性拟议的为期四年的 SCORE SC3 研究计划将重点了解近表面空间控制、非共价相互作用和手性相互作用如何确定改性纳米颗粒对模型有机反应的催化特性。与生物学上重要的转化（烯烃还原和异构化）相关的资金为 PI 提供夏季和学术支持，每年为 1 名学士后研究员或技术人员提供支持，化学品，这项工作涉及四项主要任务：1）用于化学选择性和区域选择性反应的近表面空间控制的金属酶模拟物。 3) 具有手性相互作用的金属酶模拟物，用于立体选择性反应。 4) 具有受控表面配体极性的金属酶模拟物。水中的重要生物学反应。研究计划将使 PI 发展基础和转化研究技能，成为纳米材料结构控制、材料表征和生物重要转化的金属酶模拟方面的独立专家，同时，该项目将提供研究生（硕士水平，2 名学生/名）。年）和本科生（4 名学生/年）在纳米技术方面拥有独特且令人兴奋的研究机会。通过注册现有的研究型课程，学生将有机会参与跨学科研究项目。在该项目的各个方面进行合作 - 从开始，从基本纳米颗粒材料合成开始，到最终完成他们还将积极培养批判性分析现有信息以及分析、解释和呈现复杂数据集的能力。招收女性和/或少数族裔学生（化学领域传统上代表性不足的群体），以促进研究和教育的平衡发展（CSULB 被指定为西班牙裔服务机构），在参与少数族裔本科研究项目（如 BUILD）方面拥有良好的记录。由 NIH 资助的建设导致多样性的基础设施）、MARC（由 NIH 资助的少数民族获得研究职业）、RISE（由 NIH 资助的科学增强研究计划）、BRIDGES（桥梁）除了目前在 CSULB 提供的 LSAMP（由 NSF 资助的路易斯·斯托克斯少数族裔参与计划）之外，还提供由 NIH 资助的学士学位）。