Amphiphilic Heterografted Molecular Bottlebrushes with Tertiary Amine‐Containing Side Chains as Efficient and Robust pH‐Responsive Emulsifiers

Abstract

By combining the unique characteristics of molecular bottlebrushes (MBBs) and the properties of stimuli‐responsive polymers, we show that MBBs with randomly grafted poly(n‐butyl acrylate) and pH‐responsive poly(2‐(N,N‐diethylamino)ethyl methacrylate) (PDEAEMA) side chains are efficient and robust pH‐responsive emulsifiers. Water‐in‐toluene emulsions were formed at pH 4.0 and disrupted by increasing the pH to 10.0. The emulsion generation and disruption was reversible over the ten cycles investigated, and the bottlebrushes remained intact. The exceptional emulsion stability stemmed from the high interfacial binding energy of MBBs, imparted by their large molecular size and Janus architecture at the interface, as evidenced by the interfacial jamming and wrinkling of the assemblies upon reducing the interfacial area. At pH 10.0, PDEAEMA became water‐insoluble, and the MBBs desorbed from the interface, causing de‐emulsification. Consequently, we have shown that the judicious design of MBBs can generate properties of particle emulsifiers from their large size, while the responsiveness of the MBBs enables more potential applications.

Document Details

Document Type
Pub Defense Publication
Publication Date
Nov 27, 2023
Source ID
10.1002/ange.202315424

Entities

People

  • Bin Zhao
  • Michael T. Kelly
  • Thomas Paul Russell
  • Zhan Chen

Organizations

  • Army Research Office
  • Lawrence Berkeley National Laboratory
  • National Science Foundation
  • University of Massachusetts
  • University of Tennessee

Tags

Fields of Study

  • Chemistry

Readers

  • Aquatic Ecology
  • Computer Networking
  • Polymer Science and Technology