Chirality transfer from a 3D macro shape to the molecular level by controlling asymmetric secondary flows.

Autor: Sevim S; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, 8093, Zurich, Switzerland.; Multi-Scale Robotics Lab, ETH Zurich, Tannenstrasse 3, CH-8092, Zurich, Switzerland., Sorrenti A; Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, 8093, Zurich, Switzerland. asorrenti@ub.edu.; Departament de Química Inorgànica i Orgànica (Secció de Química Orgànica), University of Barcelona (UB), 08028, Barcelona, Spain. asorrenti@ub.edu.; Institut de Química Teòrica i Computacional, University of Barcelona (UB), 08028, Barcelona, Spain. asorrenti@ub.edu., Vale JP; Transport Phenomena Research Centre (CEFT), Engineering Faculty of Porto University, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal.; Associate Laboratory in Chemical Engineering (ALICE), Engineering Faculty of Porto University, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal., El-Hachemi Z; Departament de Química Inorgànica i Orgànica (Secció de Química Orgànica), University of Barcelona (UB), 08028, Barcelona, Spain., Pané S; Multi-Scale Robotics Lab, ETH Zurich, Tannenstrasse 3, CH-8092, Zurich, Switzerland., Flouris AD; FAME Laboratory, Department of Exercise Science, University of Thessaly, Volos, Greece., Mayor TS; Transport Phenomena Research Centre (CEFT), Engineering Faculty of Porto University, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal. tiago.sottomayor@fe.up.pt.; Associate Laboratory in Chemical Engineering (ALICE), Engineering Faculty of Porto University, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal. tiago.sottomayor@fe.up.pt., Puigmartí-Luis J; Institut de Química Teòrica i Computacional, University of Barcelona (UB), 08028, Barcelona, Spain. josep.puigmarti@ub.edu.; Departament de Ciència dels Materials i Química Física, University of Barcelona (UB), 08028, Barcelona, Spain. josep.puigmarti@ub.edu.; Institució Catalana de Recerca i Estudis Avançats (ICREA), Pg. Lluís Companys 23, 08010, Barcelona, Spain. josep.puigmarti@ub.edu.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2022 Apr 01; Vol. 13 (1), pp. 1766. Date of Electronic Publication: 2022 Apr 01.
DOI: 10.1038/s41467-022-29425-y
Abstrakt: Homochirality is a fundamental feature of living systems, and its origin is still an unsolved mystery. Previous investigations showed that external physical forces can bias a spontaneous symmetry breaking process towards deterministic enantioselection. But can the macroscopic shape of a reactor play a role in chiral symmetry breaking processes? Here we show an example of chirality transfer from the chiral shape of a 3D helical channel to the chirality of supramolecular aggregates, with the handedness of the helical channel dictating the direction of enantioselection in the assembly of an achiral molecule. By combining numerical simulations of fluid flow and mass transport with experimental data, we demonstrated that the chiral information is transferred top-down thanks to the interplay between the hydrodynamics of asymmetric secondary flows and the precise spatiotemporal control of reagent concentration fronts. This result shows the possibility of controlling enantioselectively molecular processes at the nanometer scale by modulating the geometry and the operating conditions of fluidic reactors.
(© 2022. The Author(s).)
Databáze: MEDLINE