Quantum Coherence-Controlled Chemical Reactions

许多工业上重要的化学生产过程需要大量的能量输入来驱动化学反应。当这种动力通过加热化学反应物提供时，可能会发生不希望发生的副反应，降低工艺产率，并可能构成安全风险。虽然存在更多可控的功率输入，但激光等光源具有固定的波长，因此仅限于少数几个反应中使用。在这项工作中，提出了一种利用量子力学原理来设计化学反应的新方法，该方法可以重定向化学反应物的随机分子运动以促进特定的化学反应。就像催化剂一样，这将导致更高的化学反应效率。化学和量子力学的独特结合将带来一种通过设计来进行化学合成的新方法。该项目将利用芝加哥大学和阿贡国家实验室之间的密切合作，成功地实施这项多学科研究。这项研究还将通过项目期间的培训和研究，为参与其中的研究生和博士后研究人员提供教育和指导。在该项目期间开发的外联方案将促进研究和教学的整合，以及代表不足的群体的参与。电子基态反应依赖于沿反应坐标的特定振动运动的激发。然而，选择激发化学键的一个特定的振动模式，同时保持其他模式不变是具有挑战性的。拟议工作的主要智力优点是解决化学合成界面临的这一长期挑战，并开发一种反应控制机制，不仅允许化学反应的键选择性激发，而且还允许调节反应势能面。这里开发的量子相干方法将能够调节特定反应通道的反应速度加速或减速的势垒。在项目的第一阶段，我们将重点了解量子相干效应对几个关键反应参数的影响，包括反应速度、选择性和产率。在第二阶段，我们的目标是优化反应控制机制，使其适用于潜在的放大应用。这项工作将研究两个重要的化学反应，并将作为广泛的潜在应用的代表。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Many industrially important chemical production processes require significant energy input to drive the chemical reactions. When this power is provided by heating the chemical reactants, undesired side reactions can take place reducing the process yield and potentially posing a safety risk. While much more controlled power inputs exist, sources such as lasers have fixed wavelengths and so are limited to use in only a handful of reactions. In this work, a new approach is proposed to use quantum mechanical principles to design chemical reactors that can redirect random chemical reactant molecular motions to promote a specific chemical reaction. Much like a catalyst, this would result in greater chemical reactor efficiency. The unique combination of chemistry and quantum mechanics proposed would lead to a new approach for chemical synthesis by design. This project will leverage a close collaboration between the University of Chicago and Argonne National Laboratory for the successful implementation of this multidisciplinary study. This research will also contribute to the education and mentoring of graduate students and postdoctoral researchers involved through their training and research during the project. Outreach programs developed during this project will foster the integration of research and teaching, as well as the participation of underrepresented groups.Electronic ground state reactions rely on the excitation of specific vibrational motions along the reaction coordinates. However, selective excitation of one specific vibrational mode of a chemical bond while leaving the others intact is challenging. The principle intellectual merit of the proposed work is to address this long-standing challenge faced by the chemical synthesis community and develop a reaction control mechanism that not only allows bond-selective excitation of chemical reactions, but also the modulation of reaction potential energy surfaces. The quantum coherence approach developed here would enable the tuning of a particular reaction channel’s potential barrier for its reaction rate acceleration or deceleration. During the first stage of the project, we will focus on understanding the influence of the quantum coherence effects on several key reaction parameters, including the reaction rate, selectivity, and yield. In the second stage, we aim to optimize the reaction control mechanism and adapt it to potential scale-up applications. Two important chemical reactions will be studied in this work and will serve as representatives of a wide range of potential applications.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.