Direct probing of single-molecule chemiluminescent reaction dynamics under catalytic conditions in solution

• Published in: Nature communications Vol. 14; no. 1; pp. 7993 - 7
• Main Authors: Zhang, Ziqing, Dong, Jinrun, Yang, Yibo, Zhou, Yuan, Chen, Yuang, Xu, Yang, Feng, Jiandong
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 02.12.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 14/63; 639/638/11/942; 639/638/77; Active sites; Catalysts; Chemical reactions; Chemiluminescence; Heterogeneity; Humanities and Social Sciences; Kinetics; multidisciplinary; Reaction kinetics; Science; Science (multidisciplinary); Substrates
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-43640-1

Chemical reaction kinetics can be evaluated by probing dynamic changes of chemical substrates or physical phenomena accompanied during the reaction process. Chemiluminescence, a light emitting exoenergetic process, involves random reaction positions and kinetics in solution that are typically characterized by ensemble measurements with nonnegligible average effects. Chemiluminescent reaction dynamics at the single-molecule level remains elusive. Here we report direct imaging of single-molecule chemiluminescent reactions in solution and probing of their reaction dynamics under catalytic conditions. Double-substrate Michaelis–Menten type of catalytic kinetics is found to govern the single-molecule reaction dynamics in solution, and a heterogeneity is found among different catalyst particles and different catalytic sites on a single particle. We further show that single-molecule chemiluminescence imaging can be used to evaluate the thermodynamics of the catalytic system, resolving activation energy at the single-particle level. Our work provides fundamental insights into chemiluminescent reactions and offers an efficient approach for evaluating catalysts. Research into the dynamics of chemical reactions at the single-molecule level is a pivotal undertaking. Here, the authors present a direct investigation of the chemiluminescent reaction dynamics of single molecules in solution, providing spatiotemporally resolved insights into chemical reactions.