Electric Field-catalyzed Single-molecule Diels-Alder Reaction Dynamics

Overview

Journal Sci Adv

Specialties Biology
Science

Date 2021 Feb 1

PMID 33523936

Citations 24

Authors

Chen Yang

Zitong Liu

Yanwei Li

Shuyao Zhou

Chenxi Lu

Yilin Guo

Melissa Ramirez

Qingzhu Zhang

Yu Li

Zhirong Liu

K N Houk

Deqing Zhang

Xuefeng Guo

Affiliations

Soon will be listed here.

Abstract

Precise time trajectories and detailed reaction pathways of the Diels-Alder reaction were directly observed using accurate single-molecule detection on an in situ label-free single-molecule electrical detection platform. This study demonstrates the well-accepted concerted mechanism and clarifies the role of charge transfer complexes with or configurations on the reaction path. An unprecedented stepwise pathway was verified at high temperatures in a high-voltage electric field. Experiments and theoretical results revealed an electric field-catalyzed mechanism that shows the presence of a zwitterionic intermediate with one bond formation and variation of concerted and stepwise reactions by the strength of the electric field, thus establishing a previously unidentified approach for mechanistic control by electric field catalysis.

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