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

美国国家科学基金会综合催化中心（CIC）是由化学学部化学创新中心（CCI）项目资助的。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刘冲和北卡罗来纳大学教堂山分校的Alexander Miller。CIC将开发所需的基础化学，利用空间分离和时间可切换的催化剂，在单个反应器中从丰富的原料池中制备合成塑料。在CIC所做的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工厂，通过结合不同的过程来构建结构复杂的产品。相比之下，合成化学家通常在一个单独的容器中单独进行每个化学反应，要求在序列的每一步之后分离产物。CIC的目标是在合成化学催化过程的发展中模拟生物系统。在时间和空间控制的帮助下，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网络，以生产新的聚合物材料。第一阶段中心的重点是使用简单的原料，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。每个参与的校园都靠近各种行业，包括制药、商品化学和塑料制造商，这有可能促进将时空可控的催化知识转移到商业企业。计划每月举办棕包研讨会，包括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。强有力的指导计划以及与当地不同群体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方法将结合空间和时间控制，使催化过程能够从简单的构建块构建序列定义的可持续聚合物材料。为了实现时间控制，可切换催化剂将被用来控制聚合物的组成。可切换催化剂可以根据需要使用外部刺激（如光或电化学电位）激活或停用，从而可以控制活性或选择性；当在同一容器中进行另一种反应时，它们也可以受到保护。为了实现空间控制，催化剂将通过微图案和/或控制局部化学环境来分离。预催化剂的表面功能化，随着模式的发展到微观尺度，将使催化具有新的反应性和提高的产物选择性。此外，潜在的光电响应的基础材料（例如，半导体）允许可调的活性部位的反应性与外部光学或电触发器以及反应物梯度的存在。CIC将结合空间和时间控制的各个方面，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型材料。例如，从乙烯或氨基酸和CO/CO2合成特定的构建块，将与它们的聚合/共聚相结合，以获得新的、精确的图案材料。项目实例包括从氨基酸和二氧化碳直接合成多肽基材料，将CO/CO2、乙烯和乙二醇转化为可持续和可降解的顺序控制共聚物，以及将二氧化碳、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得到应用。学生将接受跨学科合作化学方面的培训，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，特别侧重于接触在科学领域代表性不足的群体的学生，将确保该项目产生进一步的影响。该奖项反映了美国国家科学基金会的法定使命，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。

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.