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（由适用提供）：基于配体覆盖金属纳米颗粒扩散原理的均质催化，最近引起了对其潜力作为酶模拟物的潜力，这是生物技术和医学研究领域中最高优先级的领域之一。特别是，简单模型纳米结构材料在增强或抵抗类似于酶类似的特定底物的添加的能力是有效投资的需求。我们的研究小组最近开发了一种新的催化系统，该系统表现出极好的活性和选择性，可用于烷烃和炔烃的异构化和/或氢化。考虑到它们的尺寸（总颗粒直径为6-8 nm），球形形状和多功能配体特性，具有活性催化金属核心这些精心设计的有机配体覆盖的纳米颗粒的可用性将特别受益于基于纳米粒子的Metaloenzyme Mimimics的进步。例如，通过在有机配体的碳氢化合物链的“尾部”中引入不同的疏水官能团，我们可以以类似于改变酶结合口袋中变化的氨基酸保留（侧基）的方式来调整近地面环境中的空间和/或非共价相互作用。这种方法将允许在表面固定配体的能力上投资通过这些分子相互作用精确调整催化选择性。拟议的四年分数SC3研究计划将集中于了解近地面空间控制，非共价相互作用以及手性相互作用如何确定改性纳米颗粒对与生物学上重要的有机转化相关的模型有机反应的催化特性（Olefin减少和异构化）。要求的资金为PI提供夏季和学术支持，支持1个后库后的研究员或技术/年/年，化学品，用品，用于研究活动的实验室消耗品以及传播的旅行费用。这项工作涉及四个主要任务：1）具有化学选择性和调节反应的近表面空间对照的金属酶模拟物。 2）金属酶模拟物具有非共价相互作用的化学选择性和调节反应。 3）金属酶模拟与立体声选择反应的手性相互作用。 4）金属酶模拟物具有受控的表面配体极性，用于水中的生物学重要反应。这研究计划将使PI能够开发基本和翻译的研究技能，成为纳米材料结构控制，材料特征和金属酶模仿生物学上重要转化的独立专家。同时，该计划将提供毕业生（M.S.级别，2名学生/年）和本科生（4名学生/年），并在纳米技术方面提供独特而激动人心的研究机会。通过参加现有研究课程的入学，将为学生提供机会成为跨学科研究计划的参与者，该研究计划将在该项目的各个方面进行合作 - 从建立开始，从基本的纳米纳米构成材料综合开始，再到完成，再到最终评估这些新金属酶模拟物的催化性能。他们还将发展智力能力，以批判性地分析现有信息，并培养在复杂数据集的分析，解释和呈现方面的熟练程度。 PI将积极积极招募女性和/或少数族裔学生，传统上代表性不足的化学群体，以增强研究和教育的平衡进步（CSULB被指定为西班牙裔服务机构）。 PI在参与少数群体的本科研究计划（例如构建（建筑基础设施）（导致NIH所付出的多样性），MARC（NIH资助的少数群体获得研究职业），RISE（NIH研究的研究计划）（NIH资助的科学增强研究计划），Bridges（以及Bridise for nih los lus funiak funitia）（以及少数人）（luis fun）（luis fun），由NSF资助），目前在CSULB中可用。