Citation: Hui Zhang, Rong Feng, Wanyi Yu, Hongbei Wei, Tianhong Wu, Peng Zhang, Wenhai Bian, Xin Li, Di Gao, Guojun Weng, Zhe Yang, Tony D. James, Xiaolong Sun. Evaluating the global thiols redox state in living cells using a reducing sulfur species responsive fluorescence switching platform[J]. Chinese Chemical Letters, ;2025, 36(4): 110528. doi: 10.1016/j.cclet.2024.110528 shu

Evaluating the global thiols redox state in living cells using a reducing sulfur species responsive fluorescence switching platform

Hui Zhang ^a ,
Rong Feng ^a ,
Wanyi Yu ^a ,
Hongbei Wei ^a ,
Tianhong Wu ^a ,
Peng Zhang ^a ,
Wenhai Bian ^a ,
Xin Li ^a ,
Di Gao ^a ,
Guojun Weng ^a ,
Zhe Yang ^a ,
Tony D. James ^{b, c} ,
Xiaolong Sun ^{a, *,}

a.
The Key Laboratory of Biomedical Information Engineering of Ministry of Education, School of Life Science and Technology, Xi’an Jiaotong University, Xi’an 710049, China
b.
Department of Chemistry, University of Bath, Bath BA2 7AY, United States
c.
School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, China

x.l.sun86@xjtu.edu.cn

Received Date: 17 July 2024
Revised Date: 30 September 2024
Accepted Date: 7 October 2024
Available Online: 10 October 2024

Figures(5)

Redox dyshomeostasis is a critical factor in the initiation of numerous diseases, making the accurate evaluation of the redox status of the cellular environment an important aspect of physiological research. However, maintaining redox homeostasis relies on a complex and dynamic physiological system involving multiple substrate-enzyme interactions, so its accurately detection remains a challenge. With this research, we developed an activable fluorescence switching platform by incorporating different conjugate acceptors to a fluorophore using ester bonds and resulting in fluorescence quenching due to donor-excited photo-induced electron transfer (d-PeT), which was confirmed through density functional theory calculations. The reaction-based probe was deployed for recognizing all major intracellular reducing sulfur species (RSS), including H₂S, cysteine (Cys), homocysteine (Hcy), glutathione (GSH), and protein free thiols. The quenched fluorescence was significantly recovered by RSS, through releasing the fluorophore and diminishing the d-PeT effect. Furthermore, the fluorescent probe was used for the sensing and imaging RSS in living cells, demonstrating good cell-permeability, low cytotoxicity, and negative correlation with reactive oxygen species content, enabling the evaluating of global thiols redox state in HepG2 cellular lines during ferroptosis processes.
- Fluorescent probe,
- Reducing sulfur species,
- Donor-excited photo-induced electron transfer,
- Thiols redox state,
- Ferroptosis
1. [1]
  G.J. McBean, M. Aslan, H.R. Griffiths, R.C. Torrão, Redox Biol. 5 (2015) 186–194. doi: 10.1016/j.redox.2015.04.004
2. [2]
  H. Sies, R.J. Mailloux, U. Jakob, Nat. Rev. Mol. Cell Biol. 25 (2024) 701–719. doi: 10.1038/s41580-024-00730-2
3. [3]
  D.A. Butterfield, M. Perluigi, Antioxid. Redox Signal. 26 (2016) 277–279.
4. [4]
  E.C. Cheung, K.H. Vousden, Nat. Rev. Cancer 22 (2022) 280–297. doi: 10.1038/s41568-021-00435-0
5. [5]
  H. Sies, V.V. Belousov, N.S. Chandel, et al., Nat. Rev. Mol. Cell Biol. 23 (2022) 499–515. doi: 10.1038/s41580-022-00456-z
6. [6]
  G.D. Ferguson, W.J. Bridge, Redox Biol. 24 (2019) 101171. doi: 10.1016/j.redox.2019.101171
7. [7]
  G. Filomeni, E. Desideri, S. Cardaci, G. Rotilio, M.R. Ciriolo, Autophagy 6 (2010) 999–1005. doi: 10.4161/auto.6.7.12754
8. [8]
  K. Ulrich, U. Jakob, Free Radical Biol. Med. 140 (2019) 14–27. doi: 10.1016/j.freeradbiomed.2019.05.035
9. [9]
  R.J. Mailloux, J.R. Treberg, Redox Biol. 8 (2016) 110–118. doi: 10.1016/j.redox.2015.12.010
10. [10]
  R. Gencheva, E.S.J. Arnér, Annu. Rev. Pharmacol. Toxicol. 62 (2022) 177–196. doi: 10.1146/annurev-pharmtox-052220-102509
11. [11]
  Z. Su, J.G. Burchfield, P. Yang, et al., Nat. Commun. 10 (2019) 5486. doi: 10.1038/s41467-019-13114-4
12. [12]
  H. Liu, F. Xu, Y. Gao, et al., Anal. Chem. 92 (2020) 8810–8818. doi: 10.1021/acs.analchem.0c00242
13. [13]
  V. Cracan, D.V. Titov, H. Shen, Z. Grabarek, V.K. Mootha, Nat. Chem. Biol. 13 (2017) 1088–1109. doi: 10.1038/nchembio.2454
14. [14]
  L.R. Knoke, L.I. Leichert, Curr. Opin. Chem. Biol. 77 (2023) 102390. doi: 10.1016/j.cbpa.2023.102390
15. [15]
  X. Chen, F. Wang, J.Y. Hyun, et al., Chem. Soc. Rev. 45 (2016) 2976–3016. doi: 10.1039/C6CS00192K
16. [16]
  H. Ren, Y. Du, X. Yang, et al., Chin. Chem. Lett. 36 (2025) 109867. doi: 10.1016/j.cclet.2024.109867
17. [17]
  C.X. Yin, K.M. Xiong, F.J. Huo, J.C. Salamanca, R.M. Strongin, Angew. Chem. Int. Ed. 56 (2017) 13188–13198. doi: 10.1002/anie.201704084
18. [18]
  Y. Yang, M. Ma, L. Shen, et al., Angew. Chem. Int. Ed. 62 (2023) e202310408. doi: 10.1002/anie.202310408
19. [19]
  T. Jin, M. Cui, D. Wu, et al., Chin. Chem. Lett. 32 (2021) 3899–3902. doi: 10.1016/j.cclet.2021.06.033
20. [20]
  Y. Zhao, Q. Hu, F. Cheng, et al., Cell Metab. 21 (2015) 777–789. doi: 10.1016/j.cmet.2015.04.009
21. [21]
  N. Patsoukis, C.D. Georgiou, Anal. Bioanal. Chem. 383 (2005) 923–929. doi: 10.1007/s00216-005-0095-5
22. [22]
  K. Umezawa, M. Yoshida, M. Kamiya, T. Yamasoba, Y. Urano, Nat. Chem. 9 (2017) 279–286. doi: 10.1038/nchem.2648
23. [23]
  H. Chen, Y. Tang, W. Lin, TrAC Trends Anal. Chem. 76 (2016) 166–181. doi: 10.1016/j.trac.2015.11.014
24. [24]
  W. Liu, C.N. Yang, Z.L. Yang, et al., Angew. Chem. Int. Ed. 62 (2023) e202304023. doi: 10.1002/anie.202304023
25. [25]
  A. Domán, É. Dóka, D. Garai, et al., Redox Biol. 60 (2023) 102617. doi: 10.1016/j.redox.2023.102617
26. [26]
  X. Feng, T. Wu, X. Sun, X. Qian, J. Am. Chem. Soc. 143 (2021) 21622–21629. doi: 10.1021/jacs.1c09895
27. [27]
  P. Zhang, X. Wang, X. Wang, et al., Anal. Chem. 95 (2023) 11953–11959. doi: 10.1021/acs.analchem.3c01518
28. [28]
  T. Wu, W. Bian, C. Wang, et al., Aggregate 4 (2023) e295. doi: 10.1002/agt2.295
29. [29]
  K.G. Fosnacht, M.D. Pluth, Chem. Rev. 124 (2024) 4124–4257. doi: 10.1021/acs.chemrev.3c00683
30. [30]
  L. Zhang, L. Zhang, X. Zhang, et al., TrAC Trends Anal. Chem. 169 (2023) 117377. doi: 10.1016/j.trac.2023.117377
31. [31]
  M. Griffith, A. Araújo, Redox Biol. 69 (2024) 103000. doi: 10.1016/j.redox.2023.103000
32. [32]
  J. van der Reest, S. Lilla, L. Zheng, S. Zanivan, E. Gottlieb, Nat. Commun. 9 (2018) 1581. doi: 10.1038/s41467-018-04003-3
33. [33]
  C. Huang, T. Jia, M. Tang, et al., J. Am. Chem. Soc. 136 (2014) 14237–14244. doi: 10.1021/ja5079656
34. [34]
  J. Duan, T. Zhang, M.J. Gaffrey, et al., Redox Biol. 36 (2020) 101649. doi: 10.1016/j.redox.2020.101649
35. [35]
  X. Jiang, B.R. Stockwell, M. Conrad, Nat. Rev. Mol. Cell Biol. 22 (2021) 266–282. doi: 10.1038/s41580-020-00324-8
36. [36]
  M. Conrad, D.A. Pratt, Nat. Chem. Biol. 15 (2019) 1137–1147. doi: 10.1038/s41589-019-0408-1
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