Title: Electric field–induced selective catalysis of single-molecule reaction

Authors: Xiaoyan Huang1,*, Chun Tang1,*, Jieqiong Li1,*, Li-Chuan Chen1,2,*, Jueting Zheng1, Pei Zhang1, Jiabo Le1, Ruihao Li1, Xiaohui Li1, Junyang Liu1,†, Yang Yang1, Jia Shi1, Zhaobin Chen1, Mindong Bai3, Hao-Li Zhang2, Haiping Xia1, Jun Cheng1,†, Zhong-Qun Tian1 and Wenjing Hong

Abstract:

Oriented external electric fields (OEEFs) offer a unique chance to tune catalytic selectivity by orienting the alignment of the electric field along the axis of the activated bond for a specific chemical reaction; however, they remain a key experimental challenge. Here, we experimentally and theoretically investigated the OEEF-induced selective catalysis in a two-step cascade reaction of the Diels-Alder addition followed by an aromatization process. Characterized by the mechanically controllable break junction (MCBJ) technique in the nanogap and confirmed by nuclear magnetic resonance (NMR) in bottles, OEEFs are found to selectively catalyze the aromatization reaction by one order of magnitude owing to the alignment of the electric field on the reaction axis. Meanwhile, the Diels-Alder reaction remained unchanged since its reaction axis is orthogonal to the electric fields. This orientation-selective catalytic effect of OEEFs reveals that chemical reactions can be selectively manipulated through the elegant alignment between the electric fields and the reaction axis.

Full-Link: https://advances.sciencemag.org/content/5/6/eaaw3072?