Controlled Polymerization of Acrylamide via One-Pot and One-Step Aqueous Cu(0)-Mediated Reversible-Deactivation Radical Polymerization

Zishan Li; Jing Lyu; Yinghao Li; Bei Qiu; Melissa Johnson; Hongyun Tai; Wenxin Wang

doi:10.1021/acs.macromol.3c00343

Controlled Polymerization of Acrylamide via One-Pot and One-Step Aqueous Cu(0)-Mediated Reversible-Deactivation Radical Polymerization

Macromolecules. 2023 Jun 19;56(13):5111-5116. doi: 10.1021/acs.macromol.3c00343. eCollection 2023 Jul 11.

Authors

Zishan Li¹, Jing Lyu¹, Yinghao Li¹, Bei Qiu¹, Melissa Johnson¹, Hongyun Tai², Wenxin Wang^{3

1

4}

Affiliations

¹ Charles Institute of Dermatology, School of Medicine, University College Dublin, Dublin 4 D04 V1W8, Ireland.
² School of Chemistry, Bangor University, Deiniol Road, Bangor, Gwynedd LL57 2UW, U.K.
³ Aust Hefei Institute for Advanced Research, Anhui University of Science and Technology, Hefei 232001, China.
⁴ School of Mechanical and Materials Engineering, University College Dublin, Dublin 4 D04 V1W8, Ireland.

Abstract

Copper-catalyzed controlled polymerization of acrylamide (AM) has always been a challenge, which typically exhibits low monomer conversion and broad molecular weight distribution (MWD) or requires complex/multistep reaction procedures, due to the highly active nature of the AM radical and its side reactions. To overcome the above challenges, herein, we report the successful synthesis of well-defined polyacrylamide (PAM) via a facile one-pot and one-step aqueous Cu(0)-mediated reversible-deactivation radical polymerization (RDRP). The results of this strategy show that strong deactivation control is the key for the controllability of AM RDRPs, which depends on the equilibria of polymerization and mutual conversion of different copper species. With the fast-propagating monomer AM, extra addition of Cu^II into the reaction system is an effective way to enhance deactivation. Based on this kinetically controlled strategy, well-defined PAMs with narrow molecular weight distributions (MWDs) and varied molecular weights (M_ws) were successfully achieved.