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)的哈尔滨·毛和沈浩以及达特茅斯大学(UMassD)马萨诸塞大学(UMassD)的张伟顺(音译)正在研究如何利用手性(不可重叠的镜面构型)匹配来改进催化剂设计和性能。开发效率更高的催化剂进行化学反应，对于包括合成化学、材料科学和生物医学科学在内的各个领域都具有重要意义。在拟议的研究项目中，将检查金核和涂层材料(即DNA)之间的手性匹配，以努力优化此类系统的催化效率。该研究项目旨在将DNA生物材料方面的专业知识与基于作用力的单分子生物物理(MAO)、单分子荧光和催化(Sen)以及单粒子光谱和显微镜(Chang)方面的专业知识进行协同。这门跨学科的科学预计将为多元化的研究团队提供丰富的学习环境，其中包括高中、大学和研究生成员中代表性不足的群体的成员。这些学生将通过联合研究会议以及KSU和UMassD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，在催化反应过程中，催化剂内部存在电荷转移，这可以通过匹配催化剂中的手性成分来调节。一种模块化的人工酶“coronazyme”已经被开发出来，作为检验这一假说的平台。这种冠状结构由以金纳米颗粒为核心和以DNA为涂层材料组成，每个成分都具有左旋手性或右旋手性。将手性与外圆偏振光激发相结合，可以得到性能优于前人的新型催化剂。该研究项目旨在建立这一手性匹配原则，如果成功，该原则很可能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。

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.