The Role of Hydrogen Bonds in Thermally Responsive Crystallization-Driven Template Autocatalysis

Huimin Wu; Qing-Xuan Chen; Yang Su; Zhen Chen

doi:10.1002/anie.202404838

The Role of Hydrogen Bonds in Thermally Responsive Crystallization-Driven Template Autocatalysis

Angew Chem Int Ed Engl. 2024 Apr 23:e202404838. doi: 10.1002/anie.202404838. Online ahead of print.

Authors

Huimin Wu¹, Qing-Xuan Chen¹, Yang Su², Zhen Chen³

Affiliations

¹ Tsinghua Shenzhen International Graduate School, Institute of Materials Research, CHINA.
² Tsinghua Shenzhen International Graduate School, Institute of Materials Research, Shen Zhen, CHINA.
³ Tsinghua Shenzhen International Graduate School, Institue of materials Research, University town of Shenzhen, Nanshan district, 518055, Shenzhen, CHINA.

PMID: 38654551
DOI: 10.1002/anie.202404838

Abstract

Autocatalysis has been well recognized to implicate in the emergence of life and is intrinsic to the biomolecular replication. Recently, an efficient template autocatalysis driven by solvent-free crystallization has been reported. Herein, we unveil the role of intermolecular hydrogen (H) bonds formed by amides in crystallization-driven template autocatalysis (CDTA), which involves the autocatalytic activity, template selectivity, and thermal responsiveness. We found that the thermal-induced cis-trans isomerization of amides possibly affects the H-bonding-mediated template ability of products for autocatalytic transformation. As a result, CDTA can be reversibly inhibited and activated by tuning the reaction temperatures. Our work sheds light on the significance of noncovalent H-bonding interactions in artificial self-replicators.

Keywords: Cis-trans isomerization; Hydrogen Bonds; Template autocatalysis; Thermal switching; crystallization.