Collaborative Research: Harnessing the chirality matching principle for enhanced catalytic reactivity

在化学系化学催化项目的支持下，肯特州立大学（KSU）的Harbin Mao和Hao Shen以及马萨诸塞州大学达特茅斯分校（UMassachusetts，Dartmouth）的Wei-Shun Chang正在研究如何使用手性（不可重叠的镜像配置）匹配来增强催化剂的设计和性能。开发具有更高效率的催化剂以进行化学反应将对包括合成化学、材料科学和生物医学科学在内的各种领域产生重大影响。在所提出的研究项目中，金核和涂层材料之间的手性匹配（即，DNA）将被检查，以努力优化这种系统的催化效率。该研究项目旨在将DNA生物材料的专业知识与基于力的单分子生物物理学（Mao），单分子荧光和催化（Shen）以及单粒子光谱学和显微镜（Chang）的专业知识相结合。这门跨学科的科学预计将为一个多元化的研究团队提供丰富的学习环境，该团队包括高中，大学和研究生成员中代表性不足的群体。这些学生将通过联合研究会议以及KSU和UMASS D之间的频繁访问进行密切互动。在这个研究项目中，这个高度合作的团队提出，在催化反应期间，催化剂内存在电荷转移，这可以通过匹配催化剂中的手性组分来调节。 一个模块化的人工酶，“冠酶”，已被开发作为平台来测试的假设。这种冠酶由作为核心的金纳米颗粒和作为涂层材料的DNA组成，每个组分都具有左手或右手手性。手性的匹配与外部圆偏振光激发相结合，可以产生新的催化剂，具有上级性能比他们的前辈。该研究项目旨在建立这种手性匹配原理，如果成功，可能会扩展到催化以外的领域，包括但不限于材料开发和传感应用中使用的分子识别。该奖项反映了NSF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。

With the support of the Chemical Catalysis program in the Division of Chemistry, Harbin Mao and Hao Shen of Kent State University (KSU) and Wei-Shun Chang of the University of Massachusetts, Dartmouth (UMassD), are studying how chirality (non-superimposable mirror configurations) matching can be used to enhance catalyst design and performance. Developing catalysts with better efficiency to carry out a chemical reaction would be consequential for a variety of fields including synthetic chemistry, materials science, and biomedical science. In the proposed research project, chirality matching between the gold core and the coating material (i.e., DNA) will be examined in an effort to optimize the catalytic efficiency of such systems. This research project aims to synergize expertise in DNA biomaterials with expertise in force-based single-molecule biophysics (Mao) and in single-molecule fluorescence and in catalysis (Shen), and in single particle spectroscopy and microscopy (Chang). This interdisciplinary science is expected to provide a rich learning environment for a diverse research team that includes members of underrepresented groups across its high-school, college, and graduate student members. These students will closely interact with each other via joint research meetings as well as frequent visits between KSU and UMassD.In this research project, this highly collaborative team proposes that charge transfer exists within a catalyst during a catalytic reaction, which could be modulated by matching the chiral components in the catalyst. A modular artificial enzyme, “coronazyme”, has been developed as the platform to test the hypothesis. This coronazyme consists of a gold nanoparticle as a core and DNA as a coating material, with each component assuming left-handed or right-handed chirality. The matching of the chirality in combination with external circularly polarized light excitation could yield novel catalysts with superior performances to their predecessors. The research project aims to establish this chirality matching principle, which, if successful, can likely be extended to the fields beyond catalysis, including, but not limited to, the molecular recognition employed in materials development and sensing 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.