Citation: Yuwan Lu, Xiaodan Zhang, Yuming Huang. Dual-site Se/NC specific peroxidase-like nanozyme for highly sensitive methimazole detection[J]. Chinese Chemical Letters, ;2025, 36(4): 110129. doi: 10.1016/j.cclet.2024.110129 shu

Dual-site Se/NC specific peroxidase-like nanozyme for highly sensitive methimazole detection

Key Laboratory of Eco-environments in Three Gorges Reservoir Region (Ministry of Education), College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China

ymhuang@swu.edu.cn

Received Date: 27 February 2024
Revised Date: 6 June 2024
Accepted Date: 14 June 2024
Available Online: 15 June 2024

Figures(6)

Tuning the nanozyme′s activity and specificity is very crucial for developing highly sensitive sensors for various applications. Herein, selenium-doped porous N-doped carbon skeletons (Se/NC) nanozymes with highly specific peroxidase-like activity were synthesized by a MOF-pyrolysis-doping protocol. Se doping adjusted the electronic structure of NC by introducing more vacancies, defective carbon and graphitic N, and endowed the resultant Se/NC enhanced charge transfer and substrate affinity. The Se/NC exhibited specific peroxidase-mimicking activity and could catalyze 3,3′,5,5′-tetramethylbenzidine oxidation by H₂O₂. Density functional theory (DFT) calculations and experimental trials indicated that both Se=O and C–Se–C species were the main active sites of Se/NC. The C–Se–C bond is the main catalytic active site endowing Se/NC with the property of nanozyme, while the Se=O bond effectively enhances its affinity to H₂O₂ and accelerate H₂O₂ dissociation. The Se/NC showed an approximately 185-fold increase in peroxidase-like activity compared to NC. Based on the inhibition of the peroxidase-like activity of Se/NC by methimazole, a colorimetric sensor was developed to achieve its sensitive detection with 2 nmol/L of limit of detection. It was successfully used for detecting methimazole in real samples. Current Se doping strategy simplifies the fabrication process of high performance specific nanozyme and promises great potential for environmental analysis.
- Se/NC peroxidase-like nanozyme,
- Dual active sites,
- Colorimetric assay,
- Methimazole,
- Environmental analysis
1. [1]
  W. Yang, X. Yang, L. Zhu, et al., Coord. Chem. Rev. 448 (2021) 214170. doi: 10.1016/j.ccr.2021.214170
2. [2]
  X. Cao, C. Zhu, Q. Hong, et al., Angew. Chem. Int. Ed. 62 (2023) e202302463. doi: 10.1002/anie.202302463
3. [3]
  S. Cao, Z. Zhao, Y. Zheng, et al., Adv. Mater. 34 (2022) 2200255. doi: 10.1002/adma.202200255
4. [4]
  Q. Zhou, H. Yang, X. Chen, et al., Angew. Chem. Int. Ed. 61 (2022) e202112453. doi: 10.1002/anie.202112453
5. [5]
  Y. Wei, J. Wu, Y. Wu, et al., Adv. Mater. 34 (2022) 2201736. doi: 10.1002/adma.202201736
6. [6]
  Y. Ai, Z. Hu, X. Liang, et al., Adv. Funct. Mater. 32 (2022) 211043.
7. [7]
  Q. Hong, H. Yang, Y. Fang, et al., Nat. Commun. 14 (2023) 2780. doi: 10.1038/s41467-023-38459-9
8. [8]
  C. Zhu, Q. Hong, K. Wang, et al., Chin. Chem. Lett. 35 (2024) 109560. doi: 10.1016/j.cclet.2024.109560
9. [9]
  X. Lu, S. Gao, H, Lin, et al., Natl. Sci. Rev. 9 (2022) nwac022. doi: 10.1093/nsr/nwac022
10. [10]
  Q. Chen, Y. Liu, Y. Lu, et al., J. Hazard. Mater. 422 (2022) 126929. doi: 10.1016/j.jhazmat.2021.126929
11. [11]
  G. Fang, R. Kang, S. Cai, C. Ge, Nano Today 48 (2023)101755. doi: 10.1016/j.nantod.2023.101755
12. [12]
  M. Chan, B. Chen, W. Huang, et al., Mater. Today Adv. 17 (2023) 100342. doi: 10.1016/j.mtadv.2023.100342
13. [13]
  S. Li, Y. Hou, Q. Chen, et al., ACS Appl. Mater. Interfaces 12 (2020) 2581–2590. doi: 10.1021/acsami.9b20275
14. [14]
  J. Sheng, Y. Wu, H. Ding, et al., Adv. Mater. 36 (2024) 2211210. doi: 10.1002/adma.202211210
15. [15]
  Q. Wang, C. Li, X. Wang, et al., Nano Lett. 22 (2022) 10003–10009. doi: 10.1021/acs.nanolett.2c03598
16. [16]
  L. Zuo, H. King, M.A. Hossain, et al., Chem. Biomed. Imaging 1 (2023) 760–766. doi: 10.1021/cbmi.3c00096
17. [17]
  Y. Kang, C. Li, H. Shi, et al., Chin. J. Chem. 41 (2023) 3189–3196. doi: 10.1002/cjoc.202300216
18. [18]
  W. Gao, J. He, L. Chen, et al., Nat. Commun. 14 (2023) 160. doi: 10.1038/s41467-023-35828-2
19. [19]
  Y. Sun, B. Xu, X. Pan, et al., Coord. Chem. Rev. 475 (2023) 214896. doi: 10.1016/j.ccr.2022.214896
20. [20]
  G. Wei, S. Liu, Y. Peng, H. Wei, Chin. J. Chem. 42 (2024) 1515–1522. doi: 10.1002/cjoc.202300755
21. [21]
  B. Zhang, J. Zhang, F. Zhang, et al., Adv. Funct. Mater. 30 (2020) 1906194. doi: 10.1002/adfm.201906194
22. [22]
  M.A. Ghausi, J. Xie, Q. Li, et al., Angew. Chem. Int. Ed. 57 (2018) 13135–13139. doi: 10.1002/anie.201807571
23. [23]
  Z. Chen, X. Su, J. Ding, et al., Appl. Catal. B 308 (2022) 121206. doi: 10.1016/j.apcatb.2022.121206
24. [24]
  T. Li, H. Xu, Cell Rep. Phys. Sci. 1 (2020) 100111. doi: 10.1016/j.xcrp.2020.100111
25. [25]
  F. Qiao, J. Wang, S. Ai, L. Li, Sens. Actuators B 216 (2015) 418–427. doi: 10.1016/j.snb.2015.04.074
26. [26]
  Q. Wang, T. Ina, W. Chen, et al., Sci. Bull. 65 (2020) 1743–1751. doi: 10.1016/j.scib.2020.06.020
27. [27]
  Y. Zhong, B. Li, S. Li, et al., Nano-Micro Lett. 10 (2018) 56. doi: 10.1007/s40820-018-0209-1
28. [28]
  Z.M.S.H. Khan, S.A. Khan, M. Zulfequar, Mater. Sci. Semicond. Process. 57 (2017) 190–196. doi: 10.1016/j.mssp.2016.10.022
29. [29]
  W. Qu, F. Shen, H. Zu, et al., Energy Fuels 34 (2020) 9779–9786. doi: 10.1021/acs.energyfuels.0c00759
30. [30]
  A. Nezhadali, L. Mehri, R. Shadmehri, Mater. Sci. Eng. C 85 (2018) 225–232. doi: 10.1016/j.msec.2017.05.099
31. [31]
  F. Lega, L. Contiero, G. Biancotto, R. Angeletti, Food Addit. Contam. A 30 (2013) 949–957. doi: 10.1080/19440049.2013.780212
32. [32]
  K. Kusmierek, E. Bald, Talanta 71 (2007) 2121–2125. doi: 10.1016/j.talanta.2006.08.019
33. [33]
  C. Yu, D. Qin, X. Jiang, X. Zheng, B. Deng, Microchem. J. 168 (2021) 106480. doi: 10.1016/j.microc.2021.106480
34. [34]
  A. Kutluay, M. Aslanoglu, Sens. Actuators B 171–172 (2012) 1216–1221.
35. [35]
  H. Lai, G. Li, Z. Zhang, Sens. Actuators B 380 (2023) 133325. doi: 10.1016/j.snb.2023.133325
36. [36]
  X. Liao, Y. Chen, M. Qin, et al., Talanta 117 (2013) 203–208. doi: 10.1016/j.talanta.2013.08.051
37. [37]
  G.M. Fernandes, W.R. Silva, D.N. Barreto, et al., Anal. Chim. Acta 1135 (2020) 187–203. doi: 10.1016/j.aca.2020.07.030
38. [38]
  M. Feng, X. Li, X. Zhang, Y. Huang, Trends Anal. Chem. 166 (2023) 117220. doi: 10.1016/j.trac.2023.117220
39. [39]
  Z. Wang, X. Jin, C. Zhu, et al., Adv. Mater. 33 (2021) 2104718. doi: 10.1002/adma.202104718
40. [40]
  L. Jiao, W. Xu, Y. Zhang, et al., Nano Today 35 (2020) 100971.
41. [41]
  J. Xu, Q. Liang, Z. Li, et al., Adv. Mater. 34 (2022) 2200011. doi: 10.1002/adma.202200011
42. [42]
  B. Yang, S. Liu, Y.V. Fedoseeva, et al., J. Power Sourc. 493 (2021) 229700.
43. [43]
  K. Zhang, X. Min, T. Zhang, et al., J. Hazard. Mater. 413 (2021) 125294.
44. [44]
  Z. Qiao, L. Lin, X. Yan, et al., Chem. Asian J. 15 (2020) 3620–3636. doi: 10.1002/asia.202000904
45. [45]
  C. Chen, L. Zhou, H. Zhang, et al., ACS EST Eng. 3 (2023) 248–259. doi: 10.1021/acsestengg.2c00287
46. [46]
  S. Liu, Q. Pan, J. Li, et al., ACS EST Water 2 (2022) 817–829. doi: 10.1021/acsestwater.1c00495
47. [47]
  H. Hu, J. Wang, B. Cui, et al., Angew. Chem. Int. Ed. 61 (2022) e202114441. doi: 10.1002/anie.202114441
48. [48]
  M. Wang, Z. Sun, H. Ci, et al., Angew. Chem. Int. Ed. 60 (2021) 24558–24565. doi: 10.1002/anie.202109291
49. [49]
  W. Ni, Z. Liu, Y. Zhang, et al., Adv. Mater. 33 (2020) 2003238. doi: 10.1002/adma.202003238
50. [50]
  Q. Wu, Y. Jia, Q. Liu, et al., Chem 8 (2022) 1–19. doi: 10.56028/ijbm.1.3.1
51. [51]
  X. Guo, H. Zhang, Y. Yao, et al., Appl. Catal. B 323 (2023) 122136.
52. [52]
  A.M. Chaparro, C. Maffiotte, Surf. Sci. Spectra 8 (2001) 105–116. doi: 10.1116/11.200110201
53. [53]
  L. Jiao, J. Wu, H. Zhong, et al., ACS Catal. 10 (2020) 6422–6429. doi: 10.1021/acscatal.0c01647
54. [54]
  S. Dong, Y. Dong, B. Liu, et al., Adv. Mater. 34 (2022) 2107054.
55. [55]
  J. Xiao, X. Yang, X. Zhao, et al., Biochem. Eng. J. 202 (2024) 109165.
56. [56]
  Y. Zhu, W. Wang, J. Cheng, et al., Angew. Chem. Int. Ed. 60 (2021) 9480–9488. doi: 10.1002/anie.202017152
57. [57]
  M. Ma, H. Wang, T. Zhang, et al., ACS Omega 8 (2023) 35779–35790. doi: 10.1021/acsomega.3c03287
58. [58]
  C. Zhang, C. Chen, D. Zhao, et al., Anal. Chem. 94 (2022) 3485–3493. doi: 10.1021/acs.analchem.1c04018
59. [59]
  Y. Huang, Z. Ding, Y. Li, F. Xi, J. Liu, Molecules 28 (2023) 4573. doi: 10.3390/molecules28124573
60. [60]
  A.M. Ariti, S.A. Geleto, B.T. Gutema, et al., Sens. Bio-Sen. Res. 42 (2023) 100595.
61. [61]
  H. Liu, Z. Gao, H. Yan, et al., Sci. China Chem. 66 (2023) 2590–2599. doi: 10.1007/s11426-023-1677-4
62. [62]
  P. Li, Y. Feng, D. Cheng, J. Wei, J. Colloid Interface Sci. 625 (2022) 435–445. doi: 10.1080/10376178.2022.2147849
63. [63]
  S. Wang, Z. Li, M. Xia, et al., Chem. Res. Chin. Univ. 6 (2023) 907–914. doi: 10.1007/s40242-022-2259-7
64. [64]
  Z. Wang, J. Liu, M. Feng, et al., Chem. Eng. J. 470 (2023) 144020.
65. [65]
  H. Wang, W. Bao, M.T. Sarwar, et al., Inorg. Chem. 62 (2023) 8418–8427. doi: 10.1021/acs.inorgchem.3c01047
66. [66]
  Y. Ma, M. Zhang, J. Wu, et al., . Small 19 (2023) 2300883.
67. [67]
  L. Gao, J. Zhuang, L. Nie, et al., Nat. Nanotechnol. 2 (2007) 577–583. doi: 10.1038/nnano.2007.260
68. [68]
  Y. Wang, T. Li, H. Wei, Anal. Chem. 95 (2023) 10105–10109. doi: 10.1021/acs.analchem.3c01830
69. [69]
  X. Li, H. Zhu, P. Liu, et al., Trends Anal. Chem. 143 (2021) 116379.
70. [70]
  S. Lin, Y. Zhang, W. Cao, et al., Dalton Trans. 48 (2019) 1993–1999. doi: 10.1039/c8dt04499f
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