Abstract
Our ability to synthesize life-inspired systems and materials is intimately connected to our understanding of the interplay between reactions, diffusion, phase separation, and self-assembly. The interaction between non-linear reactions (autocatalysis) and liquid-liquid phase separation is particularly interesting because of the emergence of functional properties and structures through instabilities, which are hard to predict theoretically without the help of experimental model systems. In this work, we studied systems where chemical autocatalysis is coupled to complex coacervation and the formation of oil-in-water droplets. The autocatalysis is driven by a nucleophilic chain reaction and is coupled to complex coacervation through the formation of tri- and tetracationic species. Interestingly, we observed the formation of hierarchical colloids when we used reactants that can form oil droplets in addition to coacervate droplets. This work illustrates a mechanism for the formation of complex, hierarchical microstructures by kinetically controlled self-assembly regulated by non-linear chemical reaction networks.
| Original language | English |
|---|---|
| Pages (from-to) | 3666-3684 |
| Number of pages | 19 |
| Journal | Chem |
| Volume | 9 |
| Issue number | 12 |
| Early online date | 28 Sept 2023 |
| DOIs | |
| Publication status | Published - 14 Dec 2023 |
Funding
We thank Nina Bukhtiiarova for the synthesis of BODIPY FL precursor dye and Anastasia Nenashkina for the graphics design. This work was supported by the Israel Science Foundation (grant 1562/23 to S.N.S.). The theoretical analysis was performed with supported of RSF (21-13-00403). The academic leadership program “Priority-2030” is acknowledged for infrastructural support. I.P. is the incumbent of the Sharon Zuckerman research fellow chair. S.N.S. supervised the research. A.I.H. T.A.M. and S.N.S. planned the project and designed experiments. A.I.H. T.A.M. A.P. B.N. I.P. T.D. and S.N.S. performed experiments and analyzed the data. N.O. and E.V.S. performed molecular dynamics simulations and contributed to graphics design. S.N.S. wrote the manuscript with help from A.I.H. T.A.M, and B.S.S. The authors declare no competing interests. One or more of the authors of this paper self-identifies as a gender minority in their field of research.
All Science Journal Classification (ASJC) codes
- General Chemistry
- Biochemistry
- Environmental Chemistry
- General Chemical Engineering
- Biochemistry, medical
- Materials Chemistry