Metal-organic Frameworks (MOF)-based Novel Electrochemiluminescence Biosensing Platform for Quantification of H2O2 Releasing from Tumor Cells

doi:10.6023/A21050223

Abstract

In this work, a kind of high-performance electrochemiluminescence (ECL) material was obtained with the assistant of metal-organic framework (MOF) structure, which realized the highly ordered assembly of ECL molecules in MOF structure, developing a new strategy of synergistically enhanced ECL. Specifically, it combined the advantages of both the pore confinement effect and the highly ordered assembly of ECL molecules in micro/nano space to enhance the ECL intensity and reaction efficiency. The proposed MOF material (abbreviated as Zr-TCPE) with excellent ECL performance was synthesized by a simple solvothermal synthesis technique employing the non-coplanar molecule 1,1,2,2-tetrachlorophenol- (4-carboxylic benzene)ethylene (H₄TCPE) as ligand and Zr₆ clusters through coordination interaction. Zr-TCPE with the porous structure can not only promote the mass transport and electron transfer in the confined micro/nano spaces, but also reduce the nonradiative relaxation and filtering effect as the H₄TCPE ligands were fixed on the rigid metal frame, restricting the free vibration/rotation and tight packing. Compared with the H₄TCPE micro/nano crystals prepared by reprecipitation method, the ECL intensity and efficiency of the Zr-TCPE increased by 3.46 times and 17.44 times with potential from 0 V to 1.4 V at 300 mV/s in 2 mL of detection solution (containing 18 mmol/L triethylamine, pH 7.4), respectively. The ECL biosensor was constructed according to the successive assembly of (i) the Zr-TCPE as ECL material, (ii) silver nanoparticles (Ag NPs) as immobilization matrix of concanavalin A (Con A) and (iii) the Con A as a cells trapping agent, which achieved the in situ monitoring of hydrogen peroxide (H₂O₂) released from the tumor cells under the stimulative effect of phorbol 12-myristate 13-acetate (PMA). Furthermore, the ECL biosensor could rapidly distinguish cancer cells from normal cells. What is more, the ECL biosensor is also suitable for the detection of H₂O₂ released from the various tumor cells. The prepared Zr-TCPE, as the combination of strong ECL emission, easy preparation and good biocompatibility, was expected to be a kind of popular luminophors for the clinical detection of tumor cells.

Key words: metal-organic framework material, 1,1,2,2-tetrachlorophenol(4-carboxylic benzene)ethylene, ECL biosensor, tumor cell, hydrogen peroxide

Cite this article

Ni Liao, Xia Zhong, Wen-Bin Liang, Ruo Yuan, Ying Zhuo. Metal-organic Frameworks (MOF)-based Novel Electrochemiluminescence Biosensing Platform for Quantification of H₂O₂ Releasing from Tumor Cells[J]. Acta Chimica Sinica, 2021, 79(10): 1257-1264.

Export EndNote|Reference Manager|ProCite|BibTeX|RefWorks

share this article

Fig. & Tab. 6

Figure 1. The schematic diagram of the preparation of Zr-TCPE (A), the fabrication procedure of Zr-TCPE based ECL biosensor (B) and the possible response mechanism of the biosensor for H2O2 (C)

Figure 2. SEM image of Zr-TCPE (A) and the SEM-EDX elemental mapping of C, O and Zr in Zr-TCPE (B). FT-IR spectra of the H4TCPE ligands (a) and Zr-TCPE (b) (C), and XRD pattern of Zr-TCPE (D)

Figure 3. (A) FL photographs of the Zr-TCPE solution with different concentrations, the concentrations: 0 mg/mL, 10-4 mg/mL, 10-3 mg/mL, 10-2 mg/mL, 10-1 mg/mL, 1 mg/mL (from left to right). The corresponding FL photographs of the Zr-TCPE under natural sunlight (B) and 365 nm UV lamp (C). (D) The FL spectra of H4TCPE monomer (a) and Zr-TCPE (b), respectively. The ECL spectra (E) and heat map (F) of the Zr-TCPE

Figure 4. (A) The DPV curves of different electrodes. (a) Bare GCE and (b) Zr-TCPE/GCE in the PBS, (c) Zr-TCPE/GCE in N2-saturated PBS. (B) ECL transients of Zr-TCPE/GCE in PBS containing 18 mmol/L TEA under different potentials. (C) ECL response curves of H4TCPE under different states. (a) The bare GCE in acetonitrile solution containing 2.75 mmol/L H4TCPE, 18 mmol/L TEA and 0.1 mol/L (TBA)BF4, (b) TCPE crystals/GCE and (c) Zr-TCPE/GCE in PBS containing 18 mmol/L TEA. Scan rates: 300 mV/s. (D) The maximum ECL spectra of TCPE crystals (a) and Zr-TCPE (b)

Figure 5. (A) ECL-time curves of the different modified electrodes in different detection solution. (a) Bare GCE in PBS, (b) Zr-TCPE/GCE in PBS containing 18 mmol/L TEA, (c) Zr-TCPE/GCE in PBS containing 18 mmol/L TEA and 1 μg/mL PMA, (d) Zr-TCPE/GCE in PBS containing 18 mmol/L TEA, 1 μg/mL PMA and 5 μmol/L H2O2. (B) ECL responses of the proposed biosensor (Con A/Ag NPs/Zr-TCPE/GCE) to Hela cells at different concentrations

Figure 6. (A) The viability of the Hela cells after incubated with Zr-TCPE with different concentrations for 48 h. (B) The ECL-potential curves of Zr-TCPE/GCE in detection solution (PBS containing 18 mmol/L TEA) containing different substances. (a) N2-saturated detection solution, (b) air-saturated detection solution, (c) detection solution containing 5 μmol/L H2O2, (d) detection solution containing 0.5% DMSO and 5 μmol/L H2O2, (e) detection solution containing 4.3 mmol/L p-benzoquinone and 5 μmol/L H2O2

References 25

[1]	Li, S. J.; Liu, Y.; Ma, Q. Trac-Trends Anal. Chem. 2019, 110, 277. doi: 10.1016/j.trac.2018.11.019
[2]	Wang, P.; Shi, Y. H.; Zhang, S. C.; Huang, X. Y.; Zhang, J. J.; Zhang, Y. W.; Si, W. L.; Dong, X. C. Small 2019, 15, 1803791. doi: 10.1002/smll.201803791
[3]	Yan, T.; Liu, Z. H.; Song, X. Y.; Zhang, S. S. Acta Chim. Sinica 2020, 78, 657. (in Chinese) doi: 10.6023/A20040132
	(闫涛, 刘振华, 宋昕玥, 张书圣, 化学学报, 2020, 78, 657.) doi: 10.6023/A20040132
[4]	Xuan, W. J.; Xia, Y. H.; Li, T.; Wang, L. L.; Liu, Y. L.; Tan, W. H. J. Am. Chem. Soc. 2020, 142, 937. doi: 10.1021/jacs.9b10755
[5]	Hao, X. J.; Zhao, S. F.; Zhang, C. M.; Hu, F. X.; Yang, H. B.; Guo, C. X. Mater. Rep. 2021, 35, 3183. (in Chinese)
	郝喜娟, 赵沈飞, 张春媚, 胡芳馨, 杨鸿斌, 郭春显, 材料导报, 2021, 35, 3183).
[6]	Liu, G.; Ma, C.; Jin, B. K.; Chen, Z. X.; Zhu, J. J. Anal. Chem. 2018, 90, 4801. doi: 10.1021/acs.analchem.8b00194
[7]	Zhang, L. W.; Chen, Q. X.; Wang, J. Y. Acta Chim. Sinica 2020, 78, 642. (in Chinese) doi: 10.6023/A20040116
	(张留伟, 陈麒先, 王静云, 化学学报, 2020, 78, 642.) doi: 10.6023/A20040116
[8]	Jiang, T.; Sun, X. X.; Wei, L. L.; Li, M. G. Anal. Chim. Acta 2020, 1135, 132. doi: 10.1016/j.aca.2020.09.040 pmid: 33070850
[9]	Notaro, A.; Gasser, G. Chem. Soc. Rev. 2017, 46, 7317. doi: 10.1039/c7cs00356k pmid: 29027562
[10]	Würthner, F.; Saha-Möller, C. R.; Fimmel, B.; Ogi, S.; Leowanawat, P.; Schmidt, D. Chem. Rev. 2016, 116, 962. doi: 10.1021/acs.chemrev.5b00188 pmid: 26270260
[11]	Nowak-Król, A.; Shoyama, K.; Stolte, M.; Wurthner, F. Chem. Commun. 2018, 54, 13763. doi: 10.1039/C8CC07640E
[12]	Zhang, X. J.; Yuan, G. D.; Li, Q. S.; Wang, B.; Zhang, X. H.; Zhang, R. Q.; Chang, J. C.; Lee, C. S.; Lee, S. T. Chem. Mater. 2008, 20, 6945. doi: 10.1021/cm801896r
[13]	Dick, J. E.; Renault, C.; Kim, B. K.; Bard, A. J. J. Am. Chem. Soc. 2014, 136, 13546. doi: 10.1021/ja507198r
[14]	Yang, B.; Xiao, J. C.; Wong, J. I.; Guo, J.; Wu, Y. C.; Ong, L. J.; Lao, L. L.; Boey, F.; Zhang, H.; Yang, H. Y.; Zhang, Q. C. J. Phys. Chem. C 2011, 115, 7924. doi: 10.1021/jp112195k
[15]	Liu, J. L.; Tang, Z. L.; Zhuo, Y.; Chai, Y. Q.; Yuan, R. Anal. Chem. 2017, 89, 9108. doi: 10.1021/acs.analchem.7b01812
[16]	Zhao, X. C.; Zhou, W. J.; Lu, C. Anal. Chem. 2017, 89, 10078. doi: 10.1021/acs.analchem.7b02921
[17]	Suk, J.; Wu, Z. Y.; Wang, L.; Bard, A. J. J. Am. Chem. Soc. 2011, 133, 14675. doi: 10.1021/ja203731n
[18]	Lai, R. Y.; Fleming, J. J.; Merner, B. L.; Vermeij, R. J.; Bodwell, G. J.; Bard, A. J. J. Phys. Chem. A 2004, 108, 376. doi: 10.1021/jp0367981
[19]	Hu, G. B.; Xiong, C. Y.; Liang, W. B.; Zeng, X. Z.; Xu, H. L.; Yang, Y.; Yao, L. Y.; Yuan, R.; Xiao, D. R. ACS Appl. Mater. Interfaces 2018, 10, 15913. doi: 10.1021/acsami.8b05038
[20]	Dong, B. L.; Song, X. Z.; Kong, X. Q.; Wang, C.; Tang, Y. H.; Liu, Y.; Lin, W. Y. Adv. Mater. 2016, 28, 8755. doi: 10.1002/adma.201602939
[21]	Wang, F.; Lin, J.; Zhao, T. B.; Hu, D. D.; Wu, T.; Liu, Y. J. Am. Chem. Soc. 2016, 138, 7718. doi: 10.1021/jacs.6b03662
[22]	Wang, S. J.; Harris, E.; Shi, J. A.; Chen, A.; Parajuli, S.; Jing, X. H.; Miao, W. Phys. Chem. Chem. Phys. 2010, 12, 10073. doi: 10.1039/c0cp00545b
[23]	Chen, T. T.; Hu, Y. H.; Cen, Y.; Chu, X.; Lu, Y. J. Am. Chem. Soc. 2013, 135, 11595. doi: 10.1021/ja4035939
[24]	Han, Z. L.; Shu, J. N.; Jiang, Q. S.; Cui, H. Anal. Chem. 2018, 90, 6064. doi: 10.1021/acs.analchem.7b05406
[25]	Shustova, N. B.; McCarthy, B. D.; Dinca, M. J. Am. Chem. Soc. 2011, 133, 20126. doi: 10.1021/ja209327q pmid: 22074054

ECL金属-有机框架(MOF)生物传感平台用于肿瘤细胞分泌H₂O₂的测定

Metal-organic Frameworks (MOF)-based Novel Electrochemiluminescence Biosensing Platform for Quantification of H₂O₂ Releasing from Tumor Cells

RichHTML

PDF

Supporting Info.

Knowledge

Abstract

Cite this article

share this article

Fig. & Tab. 6

References 25

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Dan Wang, Bo Feng, Xiaoxin Zhang, Yanan Liu, Yan Pei, Minghua Qiao, Baoning Zong. Nitrogen-doped Carbon Pyrolyzed from ZIF-8 for Electrocatalytic Oxygen Reduction to Hydrogen Peroxide [J]. Acta Chimica Sinica, 2022, 80(6): 772-780.
[2]	Xufei Li, Baoyou Yan, Weiqiu Huang, Lipei Fu, Xianhang Sun, Aihua Lv. Research Progress in Metal-Organic Framework and Its Composites for Separation of C₂ Based on Sieving Multiple Effects [J]. Acta Chimica Sinica, 2021, 79(4): 459-471.
[3]	Gao Juyi, Du Jinghui, Zhang Wang, Zhang Baoyue, Liu Zongbin, Chen Yan, Xu Xiaoping. A Simple Fabricated Microfluidic Chip for Rapid Capture of Circulating Tumor Cells [J]. Acta Chimica Sinica, 2014, 72(1): 69-74.
[4]	Xie Wenjing, Fu Yingyi, Ma Hong, Zhang Mo, Fan Louzhen. Preparation of Fluorescent Graphene Quantum Dots as Biological Imaging Marker for Cells [J]. Acta Chimica Sinica, 2012, 70(20): 2169-2172.
[5]	Tang Kan, Tao Huijin, Jiang Xinyu. Possible Reaction between Titanium(IV) and Hydrogen Peroxide in Acidic Condition: An ab-initio Study on Its Mechanism [J]. Acta Chimica Sinica, 2012, 70(19): 2091-2096.
[6]	Li Yanxia, Duan Xiaoyong, Li Xianguo, Tang Xuli. Mechanism Study on Photodegradation of Nonylphenol in Water by Intermediate Products Analysis [J]. Acta Chimica Sinica, 2012, 70(17): 1819-1826.
[7]	Xia Qianfang, Huang Yingjuan, Yang Xue, Li Zaijun. Preparation and its Application of Novel Graphene/Gold/Functional Conducting Polymer/Hydrogen Peroxide Biosensor [J]. Acta Chimica Sinica, 2012, 70(11): 1315-1321.
[8]	LI Yan, GAO Yan-Fang, LIU Yu-Chen, ZHOU Yu, LIU Jin-Rong. Direct Electrochemistry of Hemoglobin Immobilized on Electrode Modified by Ceria [J]. Acta Chimica Sinica, 2010, 68(12): 1161-1166.
[9]	ZHANG Shi-Guo, BIAN He, XIA Dao-Hong. Theoretical Study on the Mechanism of CH₃SH with H₂O₂ under Atmospheric Conditions [J]. Acta Chimica Sinica, 2010, 68(11): 1050-1056.
[10]	CENG Wei-Feng, LI Xiao-Gong, DU Juan, LI Jian-Mei, ZHANG Beng, HU Chang-Wei, MENG Xiang-Guang. Kinetic Study on Oxidation of 1-(3,4-dimethoxyphenyl)ethanol Catalyzed by Copper(II) Complexes [J]. Acta Chimica Sinica, 2010, 68(01): 27-32.
[11]	. Electrochemical Properties of the Keggin-type Lacunary Heteropolytungstate Anion and Its Electrocatalysis for H2O2 Reduction [J]. Acta Chimica Sinica, 2009, 67(8): 795-800.
[12]	ZHANG Shu, QIU Ting, GUAN Hong-Liang, HE Chi-Ke. A New Method to Polymerize the Water Soluble Conjugated Polymer MPS-PPV and the Studies on the Fluorescence Wavelength Regulation [J]. Acta Chimica Sinica, 2009, 67(24): 2827-2832.
[13]	. Molecular Dynamics Simulation on Characteristics of Decomposition of Methane Hydrate in the Presence of Hydrogen Peroxide Solution [J]. Acta Chimica Sinica, 2009, 67(18): 2149-2154.
[14]	. New Epoxidation Process of Biological Oils and Fats and Its Mechanism [J]. Acta Chimica Sinica, 2009, 67(13): 1412-1416.
[15]	WENG Zhi-Huan ;WANG Jin-Yan ;JIAN Xi-Gao*. Synthesis and Characterization of the Phosphotungstic Reac-tion-controlled Phase-transfer Catalyst [J]. Acta Chimica Sinica, 2008, 66(3): 371-375.

ECL金属-有机框架(MOF)生物传感平台用于肿瘤细胞分泌H2O2的测定