Citation: Peng Jin, Sili Lin, Dongmei Wang, Jinsong Fan, Qingyun Liu, Kun Li. Valence-band hybridization endows the reaction specificity of AgPd nanozyme for exclusive peroxidase mimicking and improved sensing performance[J]. Chinese Chemical Letters, ;2025, 36(11): 110916. doi: 10.1016/j.cclet.2025.110916 shu

Valence-band hybridization endows the reaction specificity of AgPd nanozyme for exclusive peroxidase mimicking and improved sensing performance

Peng Jin ^{a, b, 1} ,
Sili Lin ^{b, 1} ,
Dongmei Wang ^{b, c, *,} ,
Jinsong Fan ^b ,
Qingyun Liu ^c ,
Kun Li ^{b, *,}

a.
Department of Mathematics and Physics, Luoyang Institute of Science and Technology, Luoyang 471023, China
b.
State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan Provincial Key Laboratory of Biomacromolecular Chemical Biology, Hunan University, Changsha 410082, China
c.
College of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266590, China

wangdm@sdust.edu.cn

kunli@hnu.edu.cn

Received Date: 27 September 2024
Revised Date: 29 December 2024
Accepted Date: 4 February 2025
Available Online: 4 February 2025

Figures(5)

Nanozymes, characterized by their stability, cost-effectiveness, and tunable catalytic activity, are promising alternatives to natural enzymes. However, specifically mimicking a single natural enzyme's activity presents a challenge. By exploiting the catalytic selectivity derived from the valence-band hybridization of noble metal nanoalloys, we introduce an alloying strategy to modulate the reaction specificity of metallic nanozymes. AgPd nanoalloy exhibits enhanced peroxidase-like activity and eliminated oxidase-like activity by adjusting the Ag content. The introduction of Ag changes the hybrid d band energy of the alloyed metal and inhibits the O₂ adsorption and decomposition on Pd, while improving the peroxidase mimicry by allowing for the H₂O₂ activation. By exemplifying the construction of a highly sensitive and selective colorimetric glucose detection platform with its practicality validated in serum samples, this strategy pioneers a multi-noble metal nanozyme with tailored peroxidase activity based on the chemical structure engineering and would advance the development of single-catalytic function nanozymes for building exclusively specific biosensors through reducing substrate competition.
- Reaction specificity,
- Peroxidase,
- Silver,
- Palladium,
- Nanoalloy,
- Glucose detection
1. [1]
  L.Z. Gao, J. Zhuang, L. Nie, et al., Nat. Nanotechnol. 2 (2007) 577–583. doi: 10.1038/nnano.2007.260
2. [2]
  M. Zandieh, J.W. Liu, Adv. Mater. 36 (2024) 2211041.
3. [3]
  G. Wei, S.J. Liu, Y.K. Peng, H. Wei, Chin. J. Chem. 42 (2024) 1515–1522. doi: 10.1002/cjoc.202300755
4. [4]
  M.C. Cai, Y.Q. Zhang, Z.X. Cao, W.S. Lin, N. Lu, ACS Appl. Mater. Interfaces 15 (2023) 18620–18629. doi: 10.1021/acsami.2c21854
5. [5]
  C. Wang, Y.Q. Wang, J.H. Liu, F. Li, P.P. Gai, Anal. Chem. 95 (2023) 15763–15768. doi: 10.1021/acs.analchem.3c03270
6. [6]
  J.S. Fan, X.Y. Zhang, W.L. Tan, Z.Z. Feng, K. Li, Nano Lett. 24 (2024) 7800–7808. doi: 10.1021/acs.nanolett.4c02175
7. [7]
  J.F. Chang, L. Yu, T. Hou, R.X. Hu, F. Li, Anal. Chem. 95 (2023) 4479–4485. doi: 10.1021/acs.analchem.2c05198
8. [8]
  W.L. Tan, X. Li, P. Zhang, et al., J. Colloid Interface Sci. 652 (2023) 1965–1973.
9. [9]
  T. Li, Y.T. Wang, W.L. Liu, et al., Angew. Chem. Int. Ed. 62 (2023) 202212438.
10. [10]
  T. Hou, N. Xu, X. Song, L. Yang, F. Li, Chin. Chem. Lett. 34 (2023) 107907.
11. [11]
  B.X. Liu, J.J. Liu, J.M. Pan, et al., Sens. Actuators B: Chem. 397 (2023) 134671.
12. [12]
  J.L. Guo, X.A. Liu, J.J. Zhao, et al., Chem. Sci. 14 (2023) 1742–1751. doi: 10.1039/d2sc05784k
13. [13]
  Z.H. Zhao, X.R. Shi, Z.W. Shen, et al., Chem. Eng. J. 469 (2023) 143923.
14. [14]
  J. Liu, L. Gong, H.Y. Chen, et al., ACS Appl. Nano Mater. 6 (2023) 5879–5888. doi: 10.1021/acsanm.3c00253
15. [15]
  M.L. Zhang, Y.Q. Wang, N. Li, D.Q. Zhu, F. Li, Biosens. Bioelectron. 237 (2023) 115554.
16. [16]
  H.Y. Li, S.X. Zhao, Z.X. Wang, F. Li, Talanta 278 (2024) 126490.
17. [17]
  Y.C. Du, Z.Y. Ke, J.H. Zhang, G.F. Feng, Biosens. Bioelectron. 216 (2022) 114656.
18. [18]
  Y. Xiao, W.J. Gong, M.D. Zhao, M. Zhang, N. Lu, Sens. Actuators B: Chem. 390 (2023) 134006.
19. [19]
  J.H. Wang, R.L. Huang, W. Qi, R.X. Su, Z.M. He, Chem. Eng. J. 434 (2022) 134677.
20. [20]
  Q.Q. Diao, X.Y. Chen, Z. Tang, et al., Environ. Sci. : Nano 11 (2024) 766–796. doi: 10.1039/d3en00844d
21. [21]
  J.H. Wang, S.Q. Gao, X. Wang, et al., Nano Res. 15 (2022) 2347–2354. doi: 10.1007/s12274-021-3854-5
22. [22]
  G. Wei, W.L. Liu, Y.H. Zhang, et al., Nano Lett. 24 (2024) 2289–2298. doi: 10.1021/acs.nanolett.3c04548
23. [23]
  J.D. Yi, Q.Q. Deng, Z.Q. Liu, et al., Small 19 (2023) 2301096.
24. [24]
  L.L. Jin, F.F. Cao, Y. Gao, et al., Adv. Mater. 35 (2023) 2301349.
25. [25]
  Y.Y. Yuan, X.X. Xi, T. Bao, et al., J. Anal. Test. 8 (2024) 278–287. doi: 10.1007/s41664-024-00298-y
26. [26]
  X. Li, W.L. Tan, J.S. Fan, K. Li, ACS Nano 18 (2024) 24162–24172. doi: 10.1021/acsnano.4c05516
27. [27]
  W.Y. Mi, S. Tang, S.S. Guo, H.J. Li, N. Shao, Chin. Chem. Lett. 33 (2022) 1331–1336.
28. [28]
  W.Q. Wang, Y.Y. Cui, X.L. Wei, et al., ACS Nano 18 (2024) 15845–15863. doi: 10.1021/acsnano.4c02825
29. [29]
  H.Z. Fan, R.F. Zhang, K.L. Fan, L.Z. Gao, X.Y. Yan, ACS Nano 18 (2024) 2533–2540. doi: 10.1021/acsnano.3c07680
30. [30]
  N. Singh, S.K. Naveen Kumar, M. Geethika, G. Mugesh, Angew. Chem. Int. Ed. 60 (2021) 3121–3130. doi: 10.1002/anie.202011711
31. [31]
  J.N. Li, W.Q. Liu, X.C. Wu, X.F. Gao, Biomaterials 48 (2015) 37–44. doi: 10.3991/ijoe.v11i3.4488
32. [32]
  Z.J. Zhang, X.H. Zhang, B.W. Liu, J.W. Liu, J. Am. Chem. Soc. 139 (2017) 5412–5419. doi: 10.1021/jacs.7b00601
33. [33]
  M.H. Li, J.X. Chen, W.W. Wu, Y.X. Fang, S.J. Dong, J. Am. Chem. Soc. 142 (2020) 15569–15574. doi: 10.1021/jacs.0c07273
34. [34]
  Y. Wang, G.R. Jia, X.Q. Cui, et al., Chem 7 (2021) 436–449. doi: 10.3390/photonics8100436
35. [35]
  Y.Y. Yang, X.L. Tan, Y.R. Wang, et al., Chem. Eng. J. 468 (2023) 143703.
36. [36]
  J.Y. Zhang, J.W. Liu, Nanoscale 12 (2020) 2914–2923. doi: 10.1039/c9nr10822j
37. [37]
  Y.F. Liu, X.Y. Wang, H. Wei, Analyst 145 (2020) 4388–4397. doi: 10.1039/d0an00389a
38. [38]
  S.L. Lin, W.L. Tan, P.F. Han, et al., Nano Res. 15 (2022) 9073–9081. doi: 10.1007/s12274-022-4538-5
39. [39]
  S.E. Son, P.K. Gupta, W. Hur, et al., ACS Appl. Nano Mater. 4 (2021) 8282–8291. doi: 10.1021/acsanm.1c01457
40. [40]
  G. Fang, W.F. Li, X.M. Shen, et al., Nat. Commun. 9 (2018) 129.
41. [41]
  P.F. Han, P. Jin, X. Li, et al., Appl. Catal. B 298 (2021) 120598.
42. [42]
  Y.L. Tang, X. Lv, W.X. Gou, et al., Anal. Bioanal. Chem. 414 (2022) 6611–6620. doi: 10.1007/s00216-022-04222-0
43. [43]
  X. Zhang, Q. Yang, Y.H. Lang, X. Jiang, P. Wu, Anal. Chem. 92 (2020) 12400–12406. doi: 10.1021/acs.analchem.0c02149
44. [44]
  L.P. Xiao, Y.S. Jun, B.H. Wu, et al., J. Mater. Chem. A 5 (2017) 6382–6387.
45. [45]
  X. Li, Y. Zhang, W.L. Tan, et al., Anal. Chem. 95 (2023) 2865–2873. doi: 10.1021/acs.analchem.2c04389
46. [46]
  J.P. McEldoon, A.R. Pokora, J.S. Dordick, Enzyme Microb. Technol. 17 (1995) 359–365.
47. [47]
  J.A. Pellicer, C. Lucas-Abellán, A. Serrano-Martínez, et al., J. Food Biochem. 40 (2016) 480–489. doi: 10.1111/jfbc.12229
48. [48]
  V. Brissos, D. Tavares, A.C. Sousa, M.P. Robalo, L.O. Martins, ACS Catal. 7 (2017) 3454–3465. doi: 10.1021/acscatal.6b03331
49. [49]
  W.C. Zhang, X.H. Niu, S.C. Meng, et al., Sens. Actuators B: Chem. 273 (2018) 400–407.
50. [50]
  S.W. Cai, Z. Fu, W. Xiao, et al., ACS Appl. Mater. Interfaces 12 (2020) 11616–11624. doi: 10.1021/acsami.9b21621
51. [51]
  H.Z. Fan, Y.Y. Li, J.B. Liu, et al., ACS Appl. Mater. Interfaces 11 (2019) 45416–45426. doi: 10.1021/acsami.9b16286
52. [52]
  Y. Liu, D.L. Purich, C.C. Wu, et al., J. Am. Chem. Soc. 137 (2015) 14952–14958. doi: 10.1021/jacs.5b08533
53. [53]
  Q. Wang, L. Zhang, C. Shang, Z. Zhang, S. Dong, Chem. Commun. 52 (2016) 5410–5413.
54. [54]
  X.W. Shen, W.Q. Liu, X.J. Gao, et al., J. Am. Chem. Soc. 137 (2015) 15882–15891. doi: 10.1021/jacs.5b10346
55. [55]
  J.Z. Li, W.L. Tan, X. Li, et al., Anal. Chem. 95 (2023) 12435–12442. doi: 10.1021/acs.analchem.3c02095
56. [56]
  S.H. Tang, L. Xu, B.J. Peng, et al., Appl. Surf. Sci. 575 (2022) 151655.
57. [57]
  S.M. Yu, X. Cheng, Y.S. Wang, et al., Nat. Commun. 13 (2022) 4737.
58. [58]
  J.W. Xu, C.C. Liang, Z.D. Gao, Y.Y. Song, Chin. Chem. Lett. 34 (2023) 107863.
59. [59]
  J.H. Zhao, H.Q. Wang, Y.H. Cai, et al., ACS Sens. 9 (2024) 1644–1655. doi: 10.1021/acssensors.4c00137
1. [1]
  Jie Ren , Hao Zong , Yaqun Han , Tianyi Liu , Shufen Zhang , Qiang Xu , Suli Wu . Visual identification of silver ornament by the structural color based on Mie scattering of ZnO spheres. Chinese Chemical Letters, 2024, 35(9): 109350-. doi: 10.1016/j.cclet.2023.109350
2. [2]
  Hailong He , Wenbing Wang , Wenmin Pang , Chen Zou , Dan Peng . Double stimulus-responsive palladium catalysts for ethylene polymerization and copolymerization. Chinese Chemical Letters, 2024, 35(7): 109534-. doi: 10.1016/j.cclet.2024.109534
3. [3]
  Junlong Tang , Yuhan Zhao , Yangbin Jin , Liren Zhang , Yuanfang Wang , Wanqing Wu , Huanfeng Jiang . Palladium-catalyzed modular biomimetic synthesis of lignans derivatives. Chinese Chemical Letters, 2025, 36(7): 110969-. doi: 10.1016/j.cclet.2025.110969
4. [4]
  Zhao Gu , Yunhui Yang , Song Ye , Congyang Wang . 2,3-Arylacylation of allenes through synergetic catalysis of palladium and N-heterocyclic carbene. Chinese Chemical Letters, 2025, 36(5): 110334-. doi: 10.1016/j.cclet.2024.110334
5. [5]
  Xiaohui Fu , Yanping Zhang , Juan Liao , Zhen-Hua Wang , Yong You , Jian-Qiang Zhao , Mingqiang Zhou , Wei-Cheng Yuan . Palladium-catalyzed enantioselective decarboxylation of vinyl cyclic carbamates: Generation of amide-based aza-1,3-dipoles and application to asymmetric 1,3-dipolar cycloaddition. Chinese Chemical Letters, 2024, 35(12): 109688-. doi: 10.1016/j.cclet.2024.109688
6. [6]
  Zhifeng CAI , Ying WU , Yanan LI , Guiyu MENG , Tianyu MIAO , Yihao ZHANG . Effective detection of malachite green by folic acid stabilized silver nanoclusters. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 983-993. doi: 10.11862/CJIC.20240394
7. [7]
  Yuwan Lu , Xiaodan Zhang , Yuming Huang . Dual-site Se/NC specific peroxidase-like nanozyme for highly sensitive methimazole detection. Chinese Chemical Letters, 2025, 36(4): 110129-. doi: 10.1016/j.cclet.2024.110129
8. [8]
  Kun Zhang , Xin-Yue Lou , Yan Wang , Weiwei Huan , Ying-Wei Yang . Emission enhancement induced by the supramolecular assembly of leggero pillar[5]arenes for the detection and separation of silver ions. Chinese Chemical Letters, 2025, 36(6): 110464-. doi: 10.1016/j.cclet.2024.110464
9. [9]
  Shuai Zhu , Mingjie Chen , Haichao Shen , Hanming Ding , Wenbo Li , Junliang Zhang . Palladium/Xu-Phos-catalyzed enantioselective arylalkoxylation reaction of γ-hydroxyalkenes at room temperature. Chinese Chemical Letters, 2024, 35(11): 109879-. doi: 10.1016/j.cclet.2024.109879
10. [10]
  Laiying Zhang , Yaxian Zhu . Exploring the Silver Family. University Chemistry, 2024, 39(9): 1-4. doi: 10.12461/PKU.DXHX202409015
11. [11]
  Yue Sun , Yingnan Zhu , Jiahang Si , Ruikang Zhang , Yalan Ji , Jinjie Fan , Yuze Dong . Glucose-activated nanozyme hydrogels for microenvironment modulation via cascade reaction in diabetic wound. Chinese Chemical Letters, 2025, 36(4): 110012-. doi: 10.1016/j.cclet.2024.110012
12. [12]
  Yu Mao , Yilin Liu , Xiaochen Wang , Shengyang Ni , Yi Pan , Yi Wang . Acylfluorination of enynes via phosphine and silver catalysis. Chinese Chemical Letters, 2024, 35(8): 109443-. doi: 10.1016/j.cclet.2023.109443
13. [13]
  Rui Wang , Yang Liang , Julius Rebek Jr. , Yang Yu . Stabilization and detection of labile reaction intermediates in supramolecular containers. Chinese Chemical Letters, 2024, 35(6): 109228-. doi: 10.1016/j.cclet.2023.109228
14. [14]
  Shaobin He , Xiaoyun Guo , Qionghua Zheng , Huanran Shen , Yuan Xu , Fenglin Lin , Jincheng Chen , Haohua Deng , Yiming Zeng , Wei Chen . Engineering nickel-supported osmium bimetallic nanozymes with specifically improved peroxidase-like activity for immunoassay. Chinese Chemical Letters, 2025, 36(4): 110096-. doi: 10.1016/j.cclet.2024.110096
15. [15]
  Wenya Jiang , Jianyu Wei , Kuan-Guan Liu . Atomically precise superatomic silver nanoclusters stabilized by O-donor ligands. Chinese Journal of Structural Chemistry, 2024, 43(9): 100371-100371. doi: 10.1016/j.cjsc.2024.100371
16. [16]
  Qing Li , Fangyu Fu , Mengyun Zhao , Yeqin Feng , Manzhou Chi , Zichen Zhao , Hongjin Lv , Guo-Yu Yang . Asymmetrically anchoring silver alkynyl cluster to the cobalt-containing polyoxometalate. Chinese Chemical Letters, 2025, 36(7): 110090-. doi: 10.1016/j.cclet.2024.110090
17. [17]
  Gongcheng Ma , Qihang Ding , Yuding Zhang , Yue Wang , Jingjing Xiang , Mingle Li , Qi Zhao , Saipeng Huang , Ping Gong , Jong Seung Kim . Palladium-free chemoselective probe for in vivo fluorescence imaging of carbon monoxide. Chinese Chemical Letters, 2024, 35(9): 109293-. doi: 10.1016/j.cclet.2023.109293
18. [18]
  Ya-Wen Zhang , Ming-Ming Gan , Li-Ying Sun , Ying-Feng Han . Supramolecular dinuclear silver(I) and gold(I) tetracarbene metallacycles and fluorescence sensing of penicillamine. Chinese Journal of Structural Chemistry, 2024, 43(9): 100356-100356. doi: 10.1016/j.cjsc.2024.100356
19. [19]
  Xin Meng , Xin-Ya Cai , Qing-Rong Ding , Shan-Shan Chen , Shu-Mei Chen , Yan-Ping He , Jian Zhang . Modifying π-conjugated coordination silver cation onto homochiral zirconium-organic cage for circularly polarized luminescence. Chinese Chemical Letters, 2025, 36(10): 110402-. doi: 10.1016/j.cclet.2024.110402
20. [20]
  Yunqiang Li , Yongxian Huang , Sinuo Li , He Huang , Zhiwei Jiao . Elaborating azaaryl alkanes enabled by photoredox/palladium dual catalyzed dialkylation of azaaryl alkenes. Chinese Chemical Letters, 2025, 36(4): 110051-. doi: 10.1016/j.cclet.2024.110051

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(24)
HTML views(3)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142