Compartmentalized Polyampholyte Microgels by Depletion Flocculation and Coacervation of Nanogels in Emulsion Droplets

Angewandte Chemie International Edition, vol. 62, pp. e202304908

Abstract

In pH-responsive drug carriers, the distribution of charges has been proven to affect delivery efficiency but is difficult to control and verify. Herein, we fabricate polyampholyte nanogel-in-microgel colloids (NiM-C) and show that the arrangement of the nanogels (NG) can easily be manipulated by adapting synthesis conditions. Positively and negatively charged pH-responsive NG are synthesized by precipitation polymerization and labelled with different fluorescent dyes. The obtained NG are integrated into microgel (MG) networks by subsequent inverse emulsion polymerization in droplet-based microfluidics. By confocal laser scanning microscopy (CLSM), we verify that depending on NG concentration, pH value and ionic strength, NiM-C with different NG arrangements are obtained, including Janus-like phase-separation of NG, statistical distribution of NG, and core-shell arrangements. Our approach is a major step towards uptake and release of oppositely charged (drug) molecules.

Authors 4

1. Hannah F. Mathews Aachen DWI - Leibniz Institute for Interactive Materials Institute of Technical and Macromolecular Chemistry

   DWI – Leibniz Institute for Interactive Materials · RWTH Aachen University

   Affiliation as printed

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University Worringerweg 2 52074 Aachen Germany

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

2. Maria I. Pieper Aachen DWI - Leibniz Institute for Interactive Materials Institute of Technical and Macromolecular Chemistry

   DWI – Leibniz Institute for Interactive Materials · RWTH Aachen University

   Affiliation as printed

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University Worringerweg 2 52074 Aachen Germany

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

3. Se‐Hyeong Jung Aachen DWI - Leibniz Institute for Interactive Materials Institute of Technical and Macromolecular Chemistry

   ETH Zurich · DWI – Leibniz Institute for Interactive Materials · RWTH Aachen University

   Affiliation as printed

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University Worringerweg 2 52074 Aachen Germany

   Laboratory for Soft Materials and Interfaces Department of Materials ETH Zürich Vladimir-Prelog-Weg 1–5/10 8093 Zürich Switzerland

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

4. Andrij Pich corresponding Aachen DWI - Leibniz Institute for Interactive Materials Institute of Technical and Macromolecular Chemistry

   Maastricht University · DWI – Leibniz Institute for Interactive Materials · RWTH Aachen University

   Affiliation as printed

   Aachen Maastricht Institute for Biobased Materials (AMIBM) Brightlands Chemelot Campus Maastricht University 6167 RD Geleen The Netherlands

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University Worringerweg 2 52074 Aachen Germany

   DWI-Leibniz Institute for Interactive Materials RWTH Aachen University Forckenbeckstr. 50 52074 Aachen Germany