Citation: Gongxi Li, Jun Jin, Junxuan Tu, Haoguo Yue, Ying Wang, Xiaohui Jia, Weiyuan Yin, Zhenglin Han, Yuxuan Deng, Chunfeng Shi, Yonggang Zhen. Intrinsically stretchable polymer semiconductors synergistically constructed by hydrogen bonds and metal coordination[J]. Chinese Chemical Letters, ;2025, 36(12): 111716. doi: 10.1016/j.cclet.2025.111716 shu

Intrinsically stretchable polymer semiconductors synergistically constructed by hydrogen bonds and metal coordination

Gongxi Li ^{a, d, 1} ,
Jun Jin ^{a, 1} ,
Junxuan Tu ^a ,
Haoguo Yue ^a ,
Ying Wang ^a ,
Xiaohui Jia ^{b, *,} ,
Weiyuan Yin ^a ,
Zhenglin Han ^a ,
Yuxuan Deng ^a ,
Chunfeng Shi ^{c, *,} ,
Yonggang Zhen ^{a, d, *,}

a.
State Key Laboratory of Organic-Inorganic Composites, College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
b.
National Demonstration Center for Experimental Life Sciences & Biotechnology Education, Beijing Normal University, Beijing 100875, China
c.
State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China
d.
State Key laboratory of Fine chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China

xhjia@bnu.edu.cn

shicf.ripp@sinopec.com

zhenyg@buct.edu.cn

Received Date: 15 April 2025
Revised Date: 12 August 2025
Accepted Date: 12 August 2025
Available Online: 13 August 2025

Figures(4)

Intrinsically stretchable semiconducting polymers play a vital role in the development of wearable electronics, featuring low-cost, large-area and high-density fabrication. Only single-stage dynamic chemical bond has been widely incorporated into polymer backbones to afford stretchability while multiple dynamic bonds have not been investigated, making a formidable challenge to achieve high stretchability without compromising charge transport properties. Herein, we synthesize a series of stretchable polymer semiconductors incorporating urethane and bipyridine units, which can provide dynamic interconnected polymer network by combination of hydrogen bonds with metal coordination, simultaneously obtaining excellent stretchability and carrier mobilities. Compared with single-stage hydrogen bonds, multiple dynamic chemical bonds constructed by 10% hydrogen bonds and 0.25 equiv. metal coordination endowed the polymer semiconductors with an 58% enhancement in carrier mobility and a two-fold increase in crack-onset strain. Notably, the polymer exhibited stable carrier mobilities parallel to the stretching direction, with 91% of initial values even under 150% strain, which is the unprecedented value for intrinsically stretchable semiconducting polymers without blending of elastomers. Therefore, the introduction of multiple dynamic bonds provides an effective and promising approach for intrinsically stretchable and high-performance polymer semiconductor.
- Hydrogen bonds,
- Metal coordination,
- Semiconducting polymer,
- Stretchability,
- Organic thin film transistor
1. [1]
  A. Chortos, J. Liu, Z. Bao, Nat. Mater. 15 (2016) 937-950. doi: 10.1038/nmat4671
2. [2]
  T. Someya, Z. Bao, G. Malliaras, Nature 540 (2016) 379-385. doi: 10.1038/nature21004
3. [3]
  J. Rogers, G. Malliaras, T. Someya, Sci. Adv. 4 (2018) eaav1889. doi: 10.1126/sciadv.aav1889
4. [4]
  D.C. Kim, H.J. Shim, W. Lee, et al., Adv. Mater. 32 (2020) 1902743. doi: 10.1002/adma.201902743
5. [5]
  J. Chen, W. Huang, D. Zheng, et al., Nat. Mater. 21 (2022) 564-571. doi: 10.1038/s41563-022-01239-9
6. [6]
  Y. Ni, L. Liu, J. Feng, et al., Chin. Chem. Lett. 34 (2023) 108419. doi: 10.1016/j.cclet.2023.108419
7. [7]
  J. Kan, S. Wang, Z. Wang, et al., Chin. Chem. Lett. 29 (2018) 1681-1684. doi: 10.1016/j.cclet.2018.07.015
8. [8]
  E.L. Melenbrink, K.M. Hilby, K. Choudhary, et al., ACS Appl. Polym. Mater. 1 (2019) 1107-1117. doi: 10.1021/acsapm.9b00115
9. [9]
  M. Matsuda, C.Y. Lin, K. Enomoto, et al., Macromolecules 56 (2023) 2348-2361. doi: 10.1021/acs.macromol.3c00109
10. [10]
  R. Peng, B. Pang, D. Hu, et al., J. Mater. Chem. C 3 (2015) 3599-3606. doi: 10.1039/C4TC02476A
11. [11]
  L.A. Galuska, W.W. McNutt, Z. Qian, et al., Macromolecules 53 (2020) 6032-6042. doi: 10.1021/acs.macromol.0c00889
12. [12]
  S. Savagatrup, X. Zhao, E. Chan, et al., Macromol. Rapid Commun. 37 (2016) 1623-1628. doi: 10.1002/marc.201600377
13. [13]
  Y. Zheng, M. Ashizawa, S. Zhang, et al., Chem. Mater. 32 (2020) 5700-5714. doi: 10.1021/acs.chemmater.0c01437
14. [14]
  J.Y. Oh, S. Rondeau-Gagne, Y.C. Chiu, et al., Nature 539 (2016) 411-415. doi: 10.1038/nature20102
15. [15]
  A. Kim, Y. Ahn, W. Li, et al., ACS Appl. Mater. Interfaces 15 (2023) 58663-58672. doi: 10.1021/acsami.3c12057
16. [16]
  S. Wang, L. Wang, S. Ren, et al., Adv. Electron. Mater. 10 (2024) 2300816. doi: 10.1002/aelm.202300816
17. [17]
  M.Y. Lee, S. Dharmapurikar, S.J. Lee, et al., Chem. Mater. 32 (2020) 1914-1924. doi: 10.1021/acs.chemmater.9b04574
18. [18]
  H.C. Wu, S. Rondeau-Gagné, Y.C. Chiu, et al., Adv. Electron. Mater. 4 (2018) 1800239. doi: 10.1002/aelm.201800239
19. [19]
  S. Chung, S.H. Kim, E. Ok, et al., Chem. Mater. 36 (2023) 74-98. doi: 10.1109/icasi57738.2023.10179526
20. [20]
  L. Laysandra, A. Njotoprajitno, S.P. Prakoso, et al., Mater. Adv. 3 (2022) 7154-7184. doi: 10.1039/d2ma00581f
21. [21]
  M. Zhu, Z. Shao, Y. Li, et al., J. Am. Chem. Soc. 146 (2024) 27429-27442. doi: 10.1021/jacs.4c07174
22. [22]
  K. Yang, Q. Li, S. Tian, et al., J. Am. Chem. Soc. 146 (2024) 10699-10707. doi: 10.1021/jacs.4c00541
23. [23]
  J.Y. Sun, X. Zhao, W.R. Illeperuma, et al., Nature 489 (2012) 133-136. doi: 10.1038/nature11409
24. [24]
  Y. Chen, A.M. Kushner, G.A. Williams, et al., Nat. Chem. 4 (2012) 467-472. doi: 10.1038/nchem.1314
25. [25]
  H. Yuk, T. Zhang, S. Lin, et al., Nat. Mater. 15 (2016) 190-196. doi: 10.1038/nmat4463
26. [26]
  H. Yue, Y. Wang, S. Luo, et al., Sci. Adv. 10 (2024) eadq0171. doi: 10.1126/sciadv.adq0171
27. [27]
  L. Li, X. Peng, D. Zhu, et al., Macromol. Chem. Phys. 224 (2023) 2300224. doi: 10.1002/macp.202300224
28. [28]
  R.J. Wojtecki, M.A. Meador, S.J. Rowan, Nat. Mater. 10 (2011) 14-27. doi: 10.1038/nmat2891
29. [29]
  L.A. Galuska, M.U. Ocheje, Z.C. Ahmad, et al., Chem. Mater. 34 (2022) 2259-2267. doi: 10.1021/acs.chemmater.1c04055
30. [30]
  H.C. Wu, F. Lissel, G.J.N. Wang, et al., Adv. Funct. Mater. 31 (2021) 2009201. doi: 10.1002/adfm.202009201
31. [31]
  R. Chen, Y. Zhou, J. Zhao, et al., Macromolecules 56 (2023) 10067-10081. doi: 10.1021/acs.macromol.3c01693
32. [32]
  V. Vazquez-Gonzalez, M.J. Mayoral, R. Chamorro, et al., J. Am. Chem. Soc. 141 (2019) 16432-16438. doi: 10.1021/jacs.9b07868
33. [33]
  G.L. Li, Z. Zhuo, B. Wang, et al., J. Am. Chem. Soc. 143 (2021) 10920-10929. doi: 10.1021/jacs.1c01161
34. [34]
  L. Zhang, Z. Liu, X. Wu, et al., Adv. Mater. 31 (2019) e1901402. doi: 10.1002/adma.201901402
35. [35]
  J. Kang, J. Mun, Y. Zheng, et al., Nat. Nanotechnol. 17 (2022) 1265-127. doi: 10.1038/s41565-022-01246-6
36. [36]
  C.H. Li, C. Wang, C. Keplinger, et al., Nat. Chem. 8 (2016) 618-624. doi: 10.1038/nchem.2492
37. [37]
  M.S. Vezie, S. Few, I. Meager, et al., Nat. Mater. 15 (2016) 746-753. doi: 10.1038/nmat4645
38. [38]
  M. Konda, S. Bhowmik, S.M. Mobin, et al., ChemistrySelect 1 (2016) 2586-2593. doi: 10.1002/slct.201600557
39. [39]
  B. Dinesh, V. Vinaya, S. Raghothama, et al., Eur. J. Org. Chem. 2013 (2013) 3590-3596. doi: 10.1002/ejoc.201300264
40. [40]
  T. Sarkar, S.A. Schneider, G. Ankonina, et al., Chem. Mater. 32 (2020) 7338-7346. doi: 10.1021/acs.chemmater.0c02199
41. [41]
  G.J.N. Wang, F. Molina-Lopez, H. Zhang, et al., Macromolecules 51 (2018) 4976-4985. doi: 10.1021/acs.macromol.8b00971
42. [42]
  H.C. Wu, S.J. Benight, A. Chortos, et al., Chem. Mater. 26 (2014) 4544-4551. doi: 10.1021/cm502271j
43. [43]
  X. Yu, L. Chen, C. Li, et al., Adv. Mater. 35 (2023) 2209896. doi: 10.1002/adma.202209896
44. [44]
  X. Wang, J. Xu, Y. Zhang, et al., Nat. Commun. 14 (2023) 4712. doi: 10.1038/s41467-023-40340-8
45. [45]
  H.W.S. Silvio Decurtins, P. Schneuwly, H.R. Oswald, Inorg. Chem. 32 (1993) 1888-1892. doi: 10.1021/ic00062a004
46. [46]
  I.D. Brown, Chem. Rev. 109 (2009) 6858–6919. doi: 10.1021/cr900053k
47. [47]
  Y. Kwon, H. Park, J.H. Oh, Chem. Mater. 35 (2023) 10672-10683. doi: 10.1021/acs.chemmater.3c02498
48. [48]
  G.J.N. Wang, L. Shaw, J. Xu, et al., Adv. Funct. Mater. 26 (2016) 7254-7262. doi: 10.1002/adfm.201602603
49. [49]
  J. Mun, G.J.N. Wang, J.Y. Oh, et al., Adv. Funct. Mater. 28 (2018) 1804222. doi: 10.1002/adfm.201804222
50. [50]
  D. Liu, J. Mun, G. Chen, et al., J. Am. Chem. Soc. 143 (2021) 11679-11689. doi: 10.1021/jacs.1c04984
51. [51]
  J. Mun, Y. Ochiai, W. Wang, et al., Nat. Commun. 12 (2021) 3572. doi: 10.1038/s41467-021-23798-2
52. [52]
  Y. Zheng, G.J.N. Wang, J. Kang, et al., Adv. Funct. Mater. 29 (2019) 1905340. doi: 10.1002/adfm.201905340
53. [53]
  G.J.N. Wang, Y. Zheng, S. Zhang, et al., Chem. Mater. 31 (2018) 6465-6475. doi: 10.1007/s10570-018-2036-4
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