Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers

Hao Wang; Wan-Su Peng; Qi Wu; Yan Zhao; Shi-Tai Wang; Yi Yang; Jin-Rong Wu; Xiao-Liang Wang; Rong-Chun Zhang

doi:10.1007/s10118-022-2742-0

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Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers

RESEARCH ARTICLE | Updated：2022-09-23

- Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers
- Chinese Journal of Polymer Science Vol. 40, Issue 10, Pages: 1297-1306(2022)
- Affiliations：
  
  a.South China Advanced Institute for Soft Matter Science and Technology (AISMST), School of Emergent Soft Matter, South China University of Technology, Guangzhou 510640, China
  b.Key Laboratory of High-Performance Polymer Materials and Technology of Ministry of Education, Department of Polymer Science and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
  c.State Key Laboratory of Polymer Materials Engineering, College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, China
  d.Suzhou Niumag Analytical Instrument Corporation, Suzhou 215151, China
  e.Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China University of Technology, Guangzhou 510640, China
- Author bio：
  
  wujinrong@scu.edu.cn (J.R.W.)
  wangxiaoliang@nju.edu.cn (X.L.W.)
  zhangcr@scut.edu.cn (R.C.Z.)
- Funds：
- DOI：10.1007/s10118-022-2742-0
  CLC：
- Received：27 January 2022，
  
  Revised：2022-3-6，
  
  Accepted：24 March 2022，
  
  Online First：27 May 2022，
  
  Published：01 October 2022
- Accepted：
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Wang, H.; Peng, W. S.; Wu, Q.; Zhao, Y.; Wang, S. T.; Yang, Y.; Wu, J. R.; Wang, X. L.; Zhang, R. C. Interplay of crosslinking structures and segmental dynamics in solid-liquid elastomers. Chinese J. Polym. Sci. 2022, 40, 1297–1306

Hao Wang, Wan-Su Peng, Qi Wu, et al. Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers[J]. Chinese Journal of Polymer Science, 2022, 40(10): 1297-1306.
Wang, H.; Peng, W. S.; Wu, Q.; Zhao, Y.; Wang, S. T.; Yang, Y.; Wu, J. R.; Wang, X. L.; Zhang, R. C. Interplay of crosslinking structures and segmental dynamics in solid-liquid elastomers. Chinese J. Polym. Sci. 2022, 40, 1297–1306 DOI： 10.1007/s10118-022-2742-0.

Hao Wang, Wan-Su Peng, Qi Wu, et al. Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers[J]. Chinese Journal of Polymer Science, 2022, 40(10): 1297-1306. DOI： 10.1007/s10118-022-2742-0.

摘要

Using a combination of rheology

proton multiple-quantum NMR and fast-field-cycling (FFC) NMR techniques

we elucidate the interplay of crosslinking structures and hierarchical segmental dynamics in the solid-liquid elastomers with variable content of dynamic boron-oxygen dative bonds

enabling the establishment of structure-dynamics-property relationship.

Abstract

There have been significant interests in recent years for incorporating dynamic bonds into polymer materials for achieving multiple functionalities

such as self-healing

recycling

stimuli-responsiveness

and so on. Nevertheless

the impact of dynamic bonds on the polymer dynamics is actually less explored. In this study

we investigate a self-healing solid-liquid elastomer (SLE)

which is a dual-crosslinked network made by coupling a permanently crosslinked polydimethylsiloxane (PDMS) network with polyborosiloxane (PBS)

via

abundant dynamic boron/oxygen dative bonds. Proton double-quantum (DQ) NMR reveals that the crosslinking degree is reduced while the structural heterogeneity of network is enhanced with increasing PBS content

i.e

increasing the content of dynamic boron/oxygen dative bonds. Rheological experiments clearly reveal two chain relaxation modes in the SLE samples with a characteristic relaxation time of around 2.1 s and 11.8 s

corresponding to the relaxation of coupled PBS and PDMS chains

respectively. The master curves obtained from variable-temperature frequency-dependent rheological experiments also reveal enhanced heterogeneity of chain relaxation with increasing PBS content. Finally

the impact of boron/oxygen dative bonds on the Rouse dynamics is further revealed by fast-field-cycling (FFC) NMR experiments

where the spin-lattice relaxation rate (

) of all SLE samples follows the same power law of

$${R}_{1} \left(\omega \right)\propto {\omega }^{-0.33}$$

http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=34728838&type=

. Nevertheless

the incorporation of PBS did slightly increase the energy barrier of Rouse dynamics. Our study well demonstrates a combined use of rheology and solid-state NMR spectroscopy can provide piercing insights into the interplay of crosslinking structures and dynamics of polymer materials.

关键词

Keywords

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