Angewandte Chemie International Edition, 25 March, 2020, DOI：http://dx.doi.org/10.1002/anie.202002904
Chiral Carbon Dots Mimicking Topoisomerase I To Mediate the Topological Rearrangement of Supercoiled DNA Enantioselectively
Prof. Feng Li Shuai Li Xiaocui Guo Yuhang Dong Dr. Chi Yao Prof. Yangping Liu Dr. Yuguang Song Dr. Xiaoli Tan Prof. Lizeng Gao Prof. Dayong Yang
Nanomaterials with enzyme‐mimetic activities are possible alternatives to natural enzymes. Mimicking enzymatic enantioselectivity remains a great challenge. Herein, we report that cysteine‐derived chiral carbon dots (CDs) can mimic topoisomerase？I to mediate topological rearrangement of supercoiled DNA enantioselectively. d ‐CDs can more effectively catalyze the topological transition of plasmid DNA from supercoiled to nicked open‐circular configuration than l ‐CDs. Experiments suggest the underlying mechanism: d ‐CDs intercalatively bind with DNA double helix more strongly than l ‐CDs; the intercalative CDs can catalyze the production of hydroxyl radicals to cleave phosphate backbone in one strand of the double helix, leading to topological rearrangement of supercoiled DNA. Molecular dynamics (MD) simulation show that the stronger affinity for hydrogen‐bond formation and hydrophobic interaction between d ‐cysteine and DNA than that of l ‐cysteine is the origin of enantioselectivity.