CCI Phase I: NSF Center for Chemistry with Electric Fields (ChEF)

美国国家科学基金会电场化学研究中心（ChEF）是由化学学部化学创新中心（CCI）项目资助的。第一阶段中心由哥伦比亚大学的拉塔·文卡塔拉曼领导。其他团队成员也来自哥伦比亚大学，包括Timothy Berkelbach， Colin Nuckolls， Tomislav Rovis和Xavier Roy。该中心面临的挑战是利用定向电场来理解、控制和操纵化学过渡态，从而改变化学反应的结果。新技术的发展扩大了可以被电场控制和操纵的反应范围。将具有合成、测量和计算专业知识的团队成员聚集在一起的战略，很好地实现了中心控制和诱导新的化学途径、加速催化和产生有机合成新范式的目标。该团队的大胆目标是通过电场控制，使传统化学催化不可能或不实用的结构、途径和中间体变得可行。更广泛的影响部分是通过与默克和哥伦比亚技术风险投资公司的强有力合作来解决的。学生有自我管理和专业发展的机会。学生共同指导，本科生也包括在团队中。该团队与纽约哈莱姆儿童区学校合作，将化学的参与扩大到K-12代表性不足的群体。化学魔术表演的发展和地铁科学与工程解决了非正式科学传播的期望。第一阶段团队在纽约的位置为STEM中代表性不足的人群提供了便利。第一阶段中心的目的是利用电场来理解、控制和操纵化学反应。这些电场可以来自纳米级电极间隙产生的外部偏置，也可以来自催化剂中策略性放置的电荷。通过外部偏置改变过渡态，是控制物质脱离平衡状态，向期望的反应性方向发展的最终证明。这项研究为控制反应中心周围的环境和电场绘制了一条路径，以加速所需的反应活性和选择性，开发出通过改变反应动力学和热力学而无法达到的反应途径和结果。CCI团队结合了合成、测量和计算方面的专业知识，并在两个跨学科研究领域开展工作，重点研究两类反应：(1)异构化和周环反应，以及(2)偶联反应。这项工作旨在提供电场如何控制反应的机制和定量理解，同时开发改变一系列反应的选择性和速率的途径，包括Claisen重排，Diels Alder环加成，碳-卤素，金属-杂原子和碳-碳键的键激活。化学是纳米科学革命的中心，本提案利用这一地位，将来自不同背景的志同道合的科学家聚集在一起，设计实验，以确定有希望的目标结构，合成这些新目标，并研究它们在电场中的性质和反应性。更广泛的影响可以通过多种方式解决。除了开发一种新的化学形式外，最重要的更广泛的影响是增加代表性不足的群体在STEM领域的参与，并帮助教育公众关于化学的优点、美丽和效用。本工作旨在改变化学在合成、材料和电场界面上的本科和研究生化学教育。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 Chemistry with Electric Fields (ChEF) is supported by the Centers for Chemical Innovation (CCI) Program of the Division of Chemistry. This Phase I Center is led by Latha Venkataraman of Columbia University. Other team members are also from Columbia and include Timothy Berkelbach, Colin Nuckolls, Tomislav Rovis, and Xavier Roy. The challenge of this center is to use directional electric fields to understand, control and manipulate chemical transition states to alter the outcomes of chemical reactions. New techniques are developed to expand the range of reactions that can be controlled and manipulated by electric fields. The strategy of bringing together team members with expertise in synthesis, measurement, and computation augers well for the Center's goal of controlling and inducing new chemical pathways, accelerating catalysis, and generating a new paradigm for organic synthesis. The bold goal of this team is to electric field control such that structures, pathways, and intermediates that are not possible or practical with traditional chemical catalysis become so. Broader impacts are addressed in part through strong collaborations with Merck and Columbia Technology Ventures. Students have opportunities for self-governance and professional development. Students are co-mentored and undergraduates are included in the team. The team partners with the Harlem Children’s Zone School in New York to broaden the participation of chemistry to K-12 underrepresented groups. Development of a Chemistry Magic Show and Subway Science and Engineering address the expectations for informal science communication. The NYC location of the Phase I team provides ready access to a population that is underrepresented in STEM. The aim of this Phase I Center is to understand, control and manipulate chemical reactions utilizing electric fields. These electric fields can originate from an external bias produced using nanoscale electrode gaps or from strategically placed charges within a catalyst. Altering transition states by an external bias is the ultimate demonstration of controlling matter away from equilibrium and toward desired reactivity. This research charts a path to controlling the environment and electric field around reaction centers to accelerate desired reactivity and selectivity, developing reaction pathways and outcomes that are otherwise inaccessible by altering reaction kinetics and thermodynamics. The CCI team combines expertise in synthesis, measurement and computation and works in two interdisciplinary research thrusts, focused on two families of reactions: (1) Isomerization and Pericyclic Reactions, and (2) Coupling Reactions. This work aims to provide a mechanistic and quantitative understanding of how electric fields can control reactions while developing routes to alter selectivity and rates in a range of reactions including the Claisen rearrangement, the Diels Alder cycloaddition, and bond activation of carbon-halogen, metal-heteroatom and carbon-carbon bonds. Chemistry is at the center of the nanoscience revolution and this proposal exploits that position bringing together like-minded scientists from a diverse set of backgrounds to design experiments to identify promising target structures, synthesize these new targets, and study their properties and reactivity in electric fields. Broader Impacts are addressed in numerous ways. In addition to developing a new form of chemistry, the overarching broader impact is to increase the participation of underrepresented groups in STEM fields and to help educate the public about the virtues, beauty, and utility of chemistry. The work aims to transform undergraduate and graduate chemical education in chemistry at the interface of synthesis, materials and electric fields.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.