Surface-confined alternating copolymerization with molecular precision by stoichiometric control

Lingbo Xing, Jie Li, Yuchen Bai, Yuxuan Lin, Lianghong Xiao, Changlin Li, Dahui Zhao, Yongfeng Wang (), Qiwei Chen (), Jing Liu () and Kai Wu ()
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Lingbo Xing: Peking University
Jie Li: Peking University
Yuchen Bai: Peking University
Yuxuan Lin: Peking University
Lianghong Xiao: Peking University
Changlin Li: Peking University
Dahui Zhao: Peking University
Yongfeng Wang: Peking University
Qiwei Chen: Peking University
Jing Liu: Peking University
Kai Wu: Peking University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Keen desires for artificial mimicry of biological polymers and property improvement of synthesized ones have triggered intensive explorations for sequence-controlled copolymerization. However, conventional synthesis faces great challenges to achieve this goal due to the strict requirements on reaction kinetics of comonomer pairs and tedious synthetic processes. Here, sequence-controlled alternating copolymerization with molecular precision is realized on surface. The stoichiometric control serves as a thermodynamic strategy to steer the polymerization selectivity, which enables the selective alternating organometallic copolymerization via intermolecular metalation of 4,4”-dibromo-p-terphenyl (P-Br) and 2,5-diethynyl-1,4-bis(phenylethynyl)benzene (A-H) with Ag adatoms on Ag(111) at P-Br: A-H = 2, as verified by scanning tunneling microscopy and density functional theory studies. In contrast, homopolymerization yield increases as the stoichiometric ratio deviates from 2. The microscopic characterizations rationalize the mechanism, providing a delicate explanation of the stoichiometry-dependent polymerization. These findings pave a way to actualizing an efficient sequence control of copolymerization by surface chemistry.

Date: 2024
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DOI: 10.1038/s41467-024-44955-3

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