Supramolecular Near‐Infrared Photocatalysts for Efficient and Oxygen‐Tolerant Aqueous RAFT Polymerization

S Siyan Guan (State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun China) Y Yue‐Yi Zhang (Academy of Interdisciplinary Studies on Intelligent Molecules Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of Chemistry Tianjin Normal University Tianjin China) S Shudi Zhang (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry) Z Zhi‐Yuan Zhang (Academy of Interdisciplinary Studies on Intelligent Molecules Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of Chemistry Tianjin Normal University Tianjin China) S Steven P. Armes (School of Mathematical and Physical Sciences, University of Sheffield, Brook Hill, Sheffield, South Yorkshire S3 7HF, U.K.) C Chunju Li (Academy of Interdisciplinary Studies on Intelligent Molecules, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry) Z Zesheng An (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry)

Abstract

ABSTRACT Near‐infrared (NIR) photocontrolled polymerization in aqueous media is promising for bioapplications. However, it typically suffers from low polymerization efficiency and requires high catalyst loadings due to the aggregated nature of the photocatalyst. Herein, we report a supramolecular strategy to overcome this limitation via host–guest complexation between an anionic photocatalyst and a cationic macrocycle. Spectroscopic and computational studies confirmed the formation of stable 1:1 host–guest complexes via synergistic electrostatic, π‐π, and hydrophobic interactions. Supramolecular complexation effectively suppresses photocatalyst aggregation and significantly enhances oxygen tolerance and reaction kinetics, enabling high‐throughput, open‐to‐air NIR‐mediated reversible addition‐fragmentation chain‐transfer (RAFT) polymerizations to be conducted in aqueous media with excellent control over molecular weight and dispersity. High conversions and low dispersities were achieved even for polymerizations conducted through thick porcine tissue barriers, demonstrating excellent NIR penetration depth. This work provides a versatile supramolecular approach to enhancing photocatalyst performance, highlighting new avenues for precision polymer synthesis under biologically relevant conditions.

Article Details

Volume / Issue Vol. 65, Issue 28
Published July 06, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (7)

S

Siyan Guan

State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun China

Y

Yue‐Yi Zhang

Academy of Interdisciplinary Studies on Intelligent Molecules Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of Chemistry Tianjin Normal University Tianjin China

S

Shudi Zhang

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry

Z

Zhi‐Yuan Zhang

Academy of Interdisciplinary Studies on Intelligent Molecules Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of Chemistry Tianjin Normal University Tianjin China

S

Steven P. Armes

School of Mathematical and Physical Sciences, University of Sheffield, Brook Hill, Sheffield, South Yorkshire S3 7HF, U.K.

C

Chunju Li

Academy of Interdisciplinary Studies on Intelligent Molecules, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry

Z

Zesheng An

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry