CCI Phase I: NSF Center for Integrated Catalysis (CIC)

CCI 第一阶段：NSF 集成催化中心 (CIC)

• 批准号: 2023955
• 负责人: Paula Diaconescu
• 金额: $ 180万
• 依托单位: University of California-Los Angeles
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2023955&HistoricalAwards=false
• 关键词: CCI; Phase; NSF; Center; Integrated

The NSF Center for Integrated Catalysis (CIC) is supported by the Centers for Chemical Innovation (CCI) Program of the Division of Chemistry. This Phase I Center is led by Paula Diaconescu of the University of California, Los Angeles. Other team members include Jeffery Byers and Dunwei Wang of Boston College, Loi Do of the University of Houston, Chong Liu of the University of California, Los Angeles, and Alexander Miller of the University of North Carolina at Chapel Hill. CIC will develop the fundamental chemistry needed to prepare synthetic plastics from pools of abundant feedstocks in a single reactor using spatially separated and temporally switchable catalysts. The inspiration for the work done in CIC comes from Nature’s remarkable ability as a chemist. Nature uses the architecture of cells to run chemical factories by combining different processes to construct structurally complex products. Synthetic chemists, in contrast, usually run each chemical reaction individually in a separate vessel, requiring product isolation after each step in the sequence. The goal of the CIC is to mimic biological systems in the development of synthetic chemical catalytic processes. Simple starting materials will be used to supply networks of multiple catalysts operating together on a single platform, with the aid of temporal and spatial control, to produce new polymeric materials. The Phase I Center focuses on using simple feedstocks such as amino acids, ethylene, carbon dioxide, and carbon monoxide. The investigators seek to develop a generally applicable platform that will help synthetic chemists to test new ideas that benefit from spatial control. The proximity of each participating campus to various industries, including pharmaceutical, commodity chemical, and plastic manufacturers, has the potential to facilitate the transfer of spatio-temporally controlled catalysis knowledge to the commercial enterprise. Monthly brown bag seminars, including sessions on business and entrepreneurship topics, are planned to help promote the career development of the students and postdoctoral scholars on the team. A strong mentoring program and existing links to local diverse populations help to ensure the recruitment and retention of underrepresented minorities in the CIC.The CIC approach will combine spatial and temporal control to enable catalytic processes that allow the construction of sequence-defined sustainable polymeric materials from simple building blocks. In order to achieve temporal control, switchable catalysts will be employed to control polymer composition. Switchable catalysts can be activated or deactivated as needed using external stimuli, such as light or electrochemical potential, enabling control over activity or selectivity; they can also be protected when another reaction is being carried out in the same vessel. In order to achieve spatial control, catalysts will be separated through micropatterning and/or controlling local chemical environments. Surface functionalization of precatalysts, along with the development of patterning down to the microscopic scale, will enable catalysis with new reactivity and improved product selectivity. Moreover, potential opto-electronic responses by the underlying materials (e.g., semiconductors) allow tunable reactivity of the active site with external optical or electrical triggers along with the presence of reactant gradients. CIC will combine aspects of spatial and temporal control to introduce a transformative approach to catalysis that converts pools of abundant feedstocks into novel materials of high complexity. For example, the synthesis of specific building blocks, from ethylene or amino acids and CO/CO2, will be coupled to their polymerization/copolymerization in order to obtain new, precisely patterned materials. Examples of projects include the direct synthesis of polypeptide-based materials from amino acids and CO2, the conversion of CO/CO2, ethylene, and ethylene glycol into sequence-controlled copolymers that are sustainable and degradable, and the conversion of CO2, ethylene, and alcohols directly to polyacrylate materials. The scientific impact of the CIC will be the introduction of a new paradigm in chemical catalysis, with applications across the catalysis community and in chemical industry. Students will be trained in interdisciplinary collaborative chemistry, benefiting from embedded research experiences at partner sites. Interactions with local communities, with a particular focus on reaching students from groups that are underrepresented in the sciences, will ensure further impact of the project.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.

NSF集成催化中心（CIC）由化学部的化学创新中心（CCI）计划提供支持。这个第一阶段中心由加州大学洛杉矶分校的Paula Diaconescu领导。其他团队成员包括波士顿学院的Jeffery Byers和Dunwei Wang，休斯顿大学的Loi Do，加州大学洛杉矶分校的Chong Liu，以及查佩尔山的北卡罗来纳州大学的亚历山大米勒。CIC将开发在单个反应器中使用空间分离和时间可切换的催化剂从丰富的原料池制备合成塑料所需的基础化学。CIC所做工作的灵感来自于大自然作为化学家的非凡能力。大自然利用细胞的结构来运行化学工厂，通过组合不同的过程来构建结构复杂的产品。相比之下，合成化学家通常在单独的容器中单独运行每个化学反应，需要在序列中的每个步骤之后分离产物。CIC的目标是在合成化学催化过程的开发中模拟生物系统。简单的起始材料将用于提供在单一平台上一起操作的多种催化剂的网络，借助于时间和空间控制，以生产新的聚合物材料。第一阶段中心专注于使用简单的原料，如氨基酸，乙烯，二氧化碳和一氧化碳。研究人员试图开发一个普遍适用的平台，帮助合成化学家测试从空间控制中受益的新想法。每个参与的校园接近各个行业，包括制药，日用化学品和塑料制造商，有可能促进时空控制催化知识向商业企业的转移。计划每月举行一次棕色袋子研讨会，包括关于商业和创业主题的会议，以帮助促进团队中学生和博士后学者的职业发展。强有力的指导计划和与当地不同人群的现有联系有助于确保在CIC中招募和保留代表性不足的少数民族。CIC方法将联合收割机空间和时间控制相结合，以实现催化过程，从而可以从简单的构建模块构建序列定义的可持续聚合物材料。为了实现时间控制，将采用可切换催化剂来控制聚合物组成。可切换催化剂可以根据需要使用外部刺激（例如光或电化学电势）活化或失活，从而能够控制活性或选择性;当在同一容器中进行另一反应时，它们也可以受到保护。为了实现空间控制，将通过微图案化和/或控制局部化学环境来分离催化剂。预催化剂的表面官能化，沿着图案化发展到微观尺度，将使催化具有新的反应性和改进的产物选择性。此外，底层材料（例如，半导体）允许活性位点与外部光或电触发沿着反应物梯度的存在的可调反应性。CIC将联合收割机结合空间和时间控制方面，引入一种变革性的催化方法，将丰富的原料池转化为高度复杂的新材料。例如，从乙烯或氨基酸和CO/CO2合成特定的结构单元将与它们的聚合/共聚反应相结合，以获得新的精确图案化的材料。项目的例子包括从氨基酸和CO2直接合成基于多肽的材料，将CO/CO2，乙烯和乙二醇转化为可持续和可降解的序列控制共聚物，以及将CO2，乙烯和醇直接转化为聚丙烯酸酯材料。CIC的科学影响将是引入化学催化的新范式，并在催化界和化学工业中应用。学生将接受跨学科合作化学的培训，受益于合作伙伴网站的嵌入式研究经验。与当地社区的互动，特别是对那些在科学领域代表性不足的群体的学生的关注，将确保该项目的进一步影响。该奖项反映了NSF的法定使命，并被认为值得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来支持。

项目成果

2-Azaaryl-1-methylpyridinium Halides: Aqueous-Soluble Activating Reagents for Efficient Amide Coupling in Water

2-氮杂芳基-1-甲基吡啶鎓卤化物：用于水中高效酰胺偶联的水溶性活化试剂

• DOI: 10.1021/acssuschemeng.2c04989
• 发表时间: 2022
• 期刊: ACS Sustainable Chemistry & Engineering
• 影响因子: 8.4
• 作者: Nguyen, Hieu D.;Tran, Thi V.;Taylor, Christopher R.;Campbell, Dylan T.;Harkins, David I.;Do, Loi H.
• 通讯作者: Do, Loi H.

Spatiotemporal control for integrated catalysis

• DOI: 10.1038/s43586-023-00207-0
• 发表时间: 2023-04
• 期刊: Nature Reviews Methods Primers
• 作者: Shijie Deng;Brandon J Jolly;James R. Wilkes;Yu Mu;J. Byers;L. Do;Alexander J. M. Miller;Dunwei Wan

The art of compartment design for synthetic catalysts

合成催化剂的隔室设计艺术

• DOI: 10.1039/d2qi02332f
• 发表时间: 2023
• 期刊: Inorganic Chemistry Frontiers
• 影响因子: 7
• 作者: Davis, Ashton R.;Liu, Chong;Diaconescu, Paula L.
• 通讯作者: Diaconescu, Paula L.

Polyketones from Carbon Dioxide and Ethylene by Integrating Electrochemical and Organometallic Catalysis

• DOI: 10.1021/acscatal.3c00769
• 发表时间: 2023-03-09
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Dodge, Henry M.;Natinsky, Benjamin S.;Miller, Alexander J. M.
• 通讯作者: Miller, Alexander J. M.