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Comprehensive Summary: Polymer dispersity (Đ) or molecular weight distribution (MWD) is a basic but vital parameter for the properties of polymeric materials. Developing new methodologies for controlling polymer MWD is emerging as a research hotspot. However, the methods to tune polymer MWD in cationic polymerization are still not well explored. Herein, we present a simple method to control the dispersity of poly(isobutyl vinyl ether) (PIBVE) by mixing two different chain transfer agents in batch visible light induced cationic RAFT polymerization. A broad dispersity range (Đ ≈ 1.16—1.80) was successfully achieved while maintaining monomodal MWD. Moreover, chain extension of PIBVE through both cationic polymerization and radical polymerization has been studied, which also provides a method to tune polymer MWD in mechanism transformation polymerization. [ABSTRACT FROM AUTHOR]

Polymer molecular weight distribution (MWD) is a key parameter of polymers. Here we present a robust method for controlling polymer MWD in controlled cationic polymerizations. A latent mediator strategy was designed and combined with temporal programming to regenerate mediators at different times during polymerization. Both the breadths and shapes of MWD curves were tuned easily by adjusting an external light source. Bimodal, trimodal, and tetramodal distributions were obtained, and the breadths could be varied from 1.06 to 2.09. Polymers with different MWDs prepared by this method had good chain end fidelity, which was demonstrated with successful chain‐extension experiments. In addition, the introduction of temporal programming with a computer‐controlled single chip for the light source opened an avenue for the use of artificial intelligence in polymer synthesis. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Polymer dispersity (Đ) or molecular weight distribution (MWD) is a basic but vital parameter for the properties of polymeric materials. Developing new methodologies for controlling polymer MWD is emerging as a research hotspot. However, the methods to tune polymer MWD in cationic polymerization are still not well explored. Herein, we present a simple method to control the dispersity of poly(isobutyl vinyl ether) (PIBVE) by mixing two different chain transfer agents in batch visible light induced cationic RAFT polymerization. A broad dispersity range (Đ ≈ 1.16—1.80) was successfully achieved while maintaining monomodal MWD. Moreover, chain extension of PIBVE through both cationic polymerization and radical polymerization has been studied, which also provides a method to tune polymer MWD in mechanism transformation polymerization. [ABSTRACT FROM AUTHOR]