High-fidelity topochemical polymerization in single crystals, polycrystals, and solution aggregates

Chongqing Yang, Jianfang Liu, Rebecca Shu Hui Khoo, Maged Abdelsamie, Miao Qi, He Li, Haiyan Mao, Sydney Hemenway, Qiang Xu, Yunfei Wang, Beihang Yu, Qingsong Zhang, Xinxin Liu, Liana M. Klivansky, Xiaodan Gu, Chenhui Zhu, Jeffrey A. Reimer, Ganglong Cui, Carolin M. Sutter-Fella, Jian Zhang, Gang Ren and Yi Liu ()
Additional contact information
Chongqing Yang: Lawrence Berkeley National Laboratory
Jianfang Liu: Lawrence Berkeley National Laboratory
Rebecca Shu Hui Khoo: Lawrence Berkeley National Laboratory
Maged Abdelsamie: Lawrence Berkeley National Laboratory
Miao Qi: Lawrence Berkeley National Laboratory
He Li: Lawrence Berkeley National Laboratory
Haiyan Mao: University of California
Sydney Hemenway: Lawrence Berkeley National Laboratory
Qiang Xu: Lawrence Berkeley National Laboratory
Yunfei Wang: Lawrence Berkeley National Laboratory
Beihang Yu: Lawrence Berkeley National Laboratory
Qingsong Zhang: Lawrence Berkeley National Laboratory
Xinxin Liu: Beijing Normal University
Liana M. Klivansky: Lawrence Berkeley National Laboratory
Xiaodan Gu: The University of Southern Mississippi
Chenhui Zhu: Lawrence Berkeley National Laboratory
Jeffrey A. Reimer: University of California
Ganglong Cui: Beijing Normal University
Carolin M. Sutter-Fella: Lawrence Berkeley National Laboratory
Jian Zhang: Lawrence Berkeley National Laboratory
Gang Ren: Lawrence Berkeley National Laboratory
Yi Liu: Lawrence Berkeley National Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Topochemical polymerization (TCP) emerges as a leading approach for synthesizing single crystalline polymers, but is traditionally restricted to transformations in solid-medium. The complexity in achieving single-crystal-to-single-crystal (SCSC) transformations due to lattice disparities and the untapped potential of performing TCP in a liquid medium with solid-state structural fidelity present unsolved challenges. Herein, by using X-rays as the primary means to overcome crystal disintegration, we reveal the details of SCSC transformation during the TCP of chiral azaquinodimethane (AQM) monomers through in situ crystallographic analysis while spotlighting a rare metastable crystalline phase. Complementary in situ investigations of powders and thin films provide critical insights into the side-chain dependent polymerization kinetics of solid-state reactions. Furthermore, we enable TCP of AQM monomers in a liquid medium via an antisolvent-reinforced aggregated state, yielding polymer nanofibers with high crystallinity akin to that of solid-state. This study testifies high structural precision of TCP performed in different states and media, offering critical insights into the synthesis of processable nanostructured polymers with desired structural integrity.

Date: 2025
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DOI: 10.1038/s41467-025-58822-2

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