Photothermy-strengthened photocatalytic activity of polydopamine-modified metal-organic frameworks for rapid therapy of bacteria-infected wounds

doi:10.1016/j.jmst.2020.05.055

Abstract

Abstract:

Herein, a metal-organic framework (MOF) was modified using polydopamine (PDA) to develop the MOF-PDA as a photoresponsive bacteria-killing agent under 660 nm light irradiation. The modification using PDA led to the production of not only more heat, but also much more¹O₂. This is because the PDA could interact with the porphyrin ring of the MOF through π-π interaction and the charge transfer between PDA and the MOFs decreases the energy of the band of hybrid nanoparticles. In addition, greater levels of hyperthermia induced by PDA modification accelerated the charge transfer, which significantly strengthened the photocatalytic performance of MOF-PDA. Furthermore, after modification, the light absorbance and water dispersibility of nanoparticles were both enhanced; both are important for the improvement of photocatalytic and photothermal properties. Consequently, MOF-PDA exhibited the highly effective antibacterial efficacy of 99.62 % and 99.97 % against Staphylococcus aureus and Escherichia coli, respectively, under 20 min 660 nm light irradiation.

Key words: Metal-organic framework, Photosensitizer, Antibacterial, Photothermal, Wound healing

Donglin Han, Yuan Li, Xiangmei Liu, Kelvin Wai Kwok Yeung, Yufeng Zheng, Zhenduo Cui, Yanqin Liang, Zhaoyang Li, Shengli Zhu, Xianbao Wang, Shuilin Wu. Photothermy-strengthened photocatalytic activity of polydopamine-modified metal-organic frameworks for rapid therapy of bacteria-infected wounds[J]. J. Mater. Sci. Technol., 2021, 62: 83-95.

Figures/Tables 13

Fig. 1. Characterization of MOF and MOF-PDA. (A) Schematic illustrating the process synthesizing MOF and MOF-PDA, as well as the structure of MOF and MOF-PDA, (B) the SEM images of the MOF, (C) the SEM images of the MOF-PDA, (D) the size distribution, (E) XRD spectra, (F) FTIR spectra of the MOF and the MOF-PDA.

Fig. 2. The morphology and water dispersibility of MOF and MOF-PDA. The TEM image and elemental mapping images of (A) MOF, (B) MOF-PDA, (C) the water dispersibility of MOF and MOF-PDA.

Fig. 3. The characterization of photothermal properties of MOF, PDA, and MOF-PDA. (A) The UV-vis spectra of MOF, MOF-PDA, and PDA, (B) the heating curves of MOF, PDA, and MOF-PDA, (C) the thermal images taken during light irradiation process of MOF, MOF-PDA, and PDA, (D) the heating and cooling curves of MOF, MOF-PDA, and PDA (660 nm, 0.7 W/cm2).

Fig. 4. The characterization of photocatalytic properties of MOF, MOF-PDA, and PDA. The detection of 1O2 at room temperature using DPBF as detector under light irradiation for (A) MOF, (B) MOF-PDA, and (C) PDA nanoparticles, the detection of 1O2 at room temperature using DPBF as detector in the dark for (D) MOF, (E) MOF-PDA, and (F) PDA nanoparticles (660 nm, 0.7 W/cm2).

Fig. 5. The mechanism of the enhanced photocatalytic properties of MOF-PDA. (A) the band energy of MOF and MOF-PDA, (B) electronic impedance spectrum, (C) photocurrent testing of MOF and MOF-PDA under light irradiation at different temperatures, Detection of the 1O2 production with DPBF as detector under light irradiation in ice bath for (D) MOF, (E) MOF-PDA, (F) PDA.

Fig. 6. Schematic illustrating the mechanism of PDA enhancing the photocatalytic property of MOF-PDA, plus the structures of MOF and MOF-PDA.

Fig. 7. Characterization of nanoparticles’ antibacterial properties. (A) the plate spreading results of the S. aureus mixed with MOF, MOF-PDA, and PDA, exposed to 660 nm light irradiation (0.7 W/cm2) or kept in dark, and statistic analysis of the spreading results, (B) the plate spreading results of the E. coli mixed with MOF, MOF-PDA and PDA, and exposed to 660 nm light irradiation (0.7 W/cm2) or kept in dark, and statistic analysis of the spreading results. (dosage: MOF-PDA, 350 ppm; MOF, 250 ppm; PDA, 100 ppm).

Fig. 8. Detection of bacterial membrane integrity using ANS and ONPG. After adding ANS, the S. aureus were mixed with (A) MOF, (B) MOF-PDA, (C) PDA and exposed to 660 nm light or kept in the dark; after adding ANS, the E. coli were mixed with (D) MOF, (E) MOF-PDA,(F) PDA and exposed to 660 nm light or kept in the dark, After the bacteria were mixed with MOF, MOF-PDA, and PDA, and exposed to 660 nm light or kept in the dark, the ONPG was added, (G) S. aureus, (H) E. coli.(-L termed as the mixture was exposed to light at room temperature; -I termed as the mixture was exposed to light in ice bath; -C termed as the mixture was kept in the dark throughout).

Fig. 9. SEM images of the different bacteria after different treatment. (dosage: MOF-PDA, 350 ppm; MOF, 250 ppm; PDA, 100 ppm).

Fig. 10. Cytotoxicity of the MOF, MOF-PDA and PDA. MTT results of the NIH 3T3 cells mixed with different nanoparticles and either exposed to light or not exposed to light for: (A) 1 day, (B) 3 day. (C) Fluorescent staining of the cells mixed with different nanoparticles and either exposed to light or kept in the dark (dosage: MOF-PDA, 350 ppm; MOF, 250 ppm; PDA, 100 ppm).

Fig. 11. The optical photographs of the infected wounds following various treatments at 2, 4, 8, 12 days. Control group, wounds covered with gauze; 3 M group, wounds covered with 3 M dressing; MOF group, wounds treated with MOF under light irradiation and covered with gauze, MOF-PDA group, wounds treated with MOF-PDA under light irradiation and covered with gauze; and then PDA group, wounds treated with PDA under light irradiation and covered with gauze.

Fig. 12. H&E staining of the tissues around wounds 2, 4, 8, 12 days after treatments.

Fig. 13. H&E staining major organs of rats 12 days after treatment.

References 57

[1]	M.X. Ma, X.M. Liu, L. Tan, Z.D. Cui, X.J. Yang, Y.Q. Liang, Z.Y. Li, Y.F. Zheng, K.W.K. Yeung, S.L. Wu, BioMater. Sci. 7 (2019) 1437-1447. DOI URL PMID
[2]	Y.J. Xi, Y. Wang, J.Y. Gao, Y.F. Xiao, J.Z. Du, ACS Nano 13 (2019) 13645-13657. DOI URL PMID
[3]	L. Piddock, Nat. Rev. Microbiol. 15 (2017) 639-640. DOI URL PMID
[4]	J.M. Zhang, Y.H. Sun, Y. Zhao, Y.L. Liu, X.H. Yao, B. Tang, R.Q. Hang, Rare Metals 36 (2019) 552-560.
[5]	X.H. Chen, Q. Wei, J.D. Hong, R. Xu, T.H. Zhou, Rare Metals 38 (2019) 413-419.
[6]	H.F. Xu, G. Zhu, B.M. Hao, J. Mater. Sci. Technol. 35 (2019) 100-108.
[7]	H. Deng, C.J. Doonan, H. Furukawa, R.B. Ferreira, J. Towne, C.B. Knobler, B. Wang, O.M. Yaghi, Science 327 (2010) 846-850. DOI URL PMID
[8]	Z.W. Ma, J.X. Zou, D. Khan, W. Zhu, C.Z. Hu, X.Q. Zeng, W.J. Ding, J. Mater. Sci. Technol. 35 (2019) 2132-2143.
[9]	B. Huang, L. Tan, X.M. Liu, J. Li, S.L. Wu, Bioact. Mater. 4 (2019) 17-21.
[10]	E.L. Zhang, S. Fu, R.X. Wang, H.X. Li, Y. Liu, Z.Q. Ma, G.K. Liu, C.S. Zhu, G.W. Qin, D. F. Chen, Rare Metals 36 (2019) 476-494.
[11]	L. Shi, L.Q. Yang, H.B. Zhang, K. Chang, G.X. Zhao, T. Kako, J.H. Ye, Appl. Catal. B 224 (2018) 60-68.
[12]	Y. Luo, X.M. Liu, L. Tan, Z.D. Cui, X.B. Feng, X.J. Yang, Y.Q. Liang, Z.Y. Li, S.L. Zhu, Y.F. Zheng, K.W.K. Yeung, C. Yang, X.B. Wang, S.L. Wu, ACS Central Sci. 5 (2019) 1591-1601.
[13]	P. Miao, G.J. Guan, H. Deng, B. Han, C. Tian, J.Y. Zhuang, Y.Y. Xu, W.Z. Liu, Z. Lin, Environ. Sci. Nano 6 (2019) 207-215.
[14]	J. Park, Q. Jiang, D.W. Feng, L.Q. Mao, H.C. Zhou, J. Am. Chem. Soc. 138 (2016) 3518-3525. DOI URL PMID
[15]	D. Feng, W. Chung, Z. Wei, Z. Gu, H. Jiang, Y. Chen, D.J. Darensbourg, H.C. Zhou, J. Am. Chem. Soc. 135 (2013) 17105-17110. DOI URL PMID
[16]	C.J. Ou, Y.W. Zhang, D. Pan, K.K. Ding, S.C. Zhang, W.J. Xu, W.J. Wang, W.L. Si, Z. Yang, X.C. Dong, Mater. Chem. Front. 3 (2019) 1786-1792. DOI URL
[17]	S.Y. Li, H. Cheng, W.X. Qiu, L. Zhang, S.S. Wan, J.Y. Zeng, X.Z. Zhang, Biomaterials 142 (2017) 149-161. DOI URL PMID
[18]	Q.L. Zou, M. Abbas, L.Y. Zhao, S.K. Li, G.Z. Shen, X.H. Yan, J. Am. Chem. Soc. 139 (2017) 1921-1927. URL PMID
[19]	A. Carangelo, A. Acquesta, T. Monetta, Bioact. Mater. 4 (2019) 71-78. DOI URL PMID
[20]	D. Sharma, W.K. Jia, F. Long, S. Pati, Q.H. Chen, Y.B. Qyang, B. Lee, C.K. Choi, F. Zhao, Bioact. Mater. 4 (2019) 142-150. URL PMID
[21]	J.J. Feng, P.P. Zhang, A.J. Wang, Q.C. Liao, J.L. Xi, J.R. Chen, New J. Chem. 36 (2012) 148-154.
[22]	S.C. Liu, J.M. Pan, J.X. Liu, Y. Ma, F.X. Qiu, L. Mei, X.W. Zeng, G.Q. Pan, Small 14 (2018), 1703968.
[23]	S.M. Yu, G.W. Li, R. Liu, D. Ma, W. Xue, Adv. Funct. Mater. 28 (2018), 1707440.
[24]	T. Li, P. Hu, J.W. Li, P.T. Huang, W.J. Tong, C.Y. Gao, Colloids Surf. A PhysicoChem. Eng. Asp. 577 (2019) 456-463.
[25]	S.X. Liu, J.L. Yang, Q. Liu, Y.J. Huang, M.Q. Kong, Q. Yang, G.G. Li, Chem. Eng. J. 363 (2019) 1-12.
[26]	J. Manna, S. Akbayrak, S. Özkar, Appl. Catal. B 208 (2017) 104-115.
[27]	J.W. Fu, Z.H. Chen, M.H. Wang, S.J. Liu, J.H. Zhang, J. Zhang, R. Han, Q. Xu, Chem. Eng. J. 259 (2015) 53-61.
[28]	F.Y. Zhao, Y.L. Ji, X.D. Weng, Y.F. Mi, C.C. Ye, Q.F. An, C.J. Gao, ACS Appl. Mater. Interfaces 8 (2016) 6693-6700.
[29]	M. Maruthapandi, M. Natan, G. Jacobi, E. Banin, J.H.T. Luong, A. Gedanken, Nanomaterials 9 (2019) 1731.
[30]	B. Gao, L.H. Chen, Y.L. Zhao, X. Yan, X.Y. Wang, C.R. Zhou, Y.F. Shi, W. Xue, Eur. Polym. J. 110 (2019) 192-201.
[31]	S. Sohrabi, S. Dehghanpour, M. Ghalkhani, J. Mater. Sci. 53 (2018) 3624-3639.
[32]	J.H. Jiang, L.P. Zhu, L.J. Zhu, H.T. Zhang, B.K. Zhu, Y.Y. Xu, ACS Appl. Mater. Interfaces 5 (2013) 12895-12904.
[33]	D.D. Wang, H.H. Wu, J.J. Zhou, P.P. Xu, C.L. Wang, R.H. Shi, H.B. Wang, H. Wang, Z. Guo, Q.W. Chen, Adv. Sci. 5 (2018), 1800287.
[34]	M. Wu, Q.T. Wang, D. Zhang, N.S. Liao, L.J. Wu, A. Huang, X.L. Liu, Colloids Surf. B Biointerfaces 141 (2016) 467-475.
[35]	D. Zhang, M. Wu, Y.Y. Zeng, L.J. Wu, Q.T. Wang, X. Han, X.L. Liu, J.F. Liu, ACS Appl. Mater. Interfaces 7 (2015) 8176-8187.
[36]	Y. Zhang, F.M. Wang, C.Q. Liu, Z.Z. Wang, L.H. Kang, Y.Y. Huang, K. Dong, J.S. Ren, X.G. Qu, ACS Nano 12 (2018) 651-661. URL PMID
[37]	K. Liu, R.R. Xing, C.J. Chen, G.Z. Shen, L.Y. Yan, Q.L. Zou, G.H. Ma, H. Möhwald, X. H. Yan, Angew. Chem. Int. Ed. 54 (2015) 500-505.
[38]	Y.W. Ren, Y.J. Han, Z.D. Cui, X.M. Liu, Z.Y. Li, S.L. Zhu, Y.Q. Liang, S.L. Wu, Bioact. Mater. 5 (2020) 201-209. DOI URL PMID
[39]	M. Tanaka, S. Hayashi, S. Eu, T. Umeyama, Y. Matano, H. Imahori, Chem. Commun. 20 (2007) 2069-2071.
[40]	W.X. Lei, K.F. Ren, T.T. Chen, X.C. Chen, B.C. Li, H. Chang, J. Ji, Adv. Mater. Interfaces 3 (2016), 1600767.
[41]	Z.L. Dong, H. Gong, M. Gao, W.W. Zhu, X.Q. Sun, L.Z. Feng, T.T. Fu, Y.G. Li, Z. Liu, Theranostics 6 (2016) 1031-1042. URL PMID
[42]	L.H. Xiao, J.H. Sun, L.B. Liu, R. Lu, H. Hu, C.G. Cheng, Y. Huang, S. Wang, ACS Appl. Mater. Interfaces 9 (2017) 5382-5391.
[43]	G. Soldan, M.A. Aljuhani, M.S. Bootharaju, L.G. AbdulHalim, M.R. Parida, A.H. Emwas, O.F. Mohammed, O.M. Bakr, Angew. Chem. Int. Ed. 55 (2016) 5749-5753.
[44]	Q. Hao, S.M. Hao, X.X. Niu, X. Li, D.M. Chen, H. Ding, Chin. J. Catal. 38 (2017) 278-286.
[45]	X. Yu, H.L. Fan, L. Wang, Z.X. Jin, Angew. Chem. Int. Ed. 53 (2014) 12600-12604.
[46]	Z.X. Gan, X.L. Wu, M. Meng, X.B. Zhu, L. Yang, P.K. Chu, ACS Nano 8 (2014) 9304-9310. DOI URL PMID
[47]	X.Z. Wang, Y.R. He, Y.W. Hu, G.R. Jin, B.C. Jiang, Y.M. Huang, Sol. Energy 170 (2018) 586-593.
[48]	L. Tan, J. Li, X.M. Liu, Z.D. Cui, X.J. Yang, S.L. Zhu, Z.Y. Li, X.B. Yuan, Y.F. Zheng, K.W.K. Yeung, H.B. Pan, X.B. Wang, S.L. Wu, Adv. Mater. 30 (2018), 1801808.
[49]	L. Schnaider, S. Brahmachari, N.W. Schmidt, B. Meusa, S. Shaham-Niv, D. Bychenko, L. Adler-Abramovich, L.J.W. Shimon, S. Kolusheva, W.F. DeGrado, E. Gazit, Nat. Commun. 8 (2017) 1-10. DOI URL PMID
[50]	T. Galbadage, D.D. Liu, L.B. Alemany, R. Pal, J.M. Tour, R.S. Gunasekera, J.D. Cirillo, ACS Nano 13 (2019) 14377-14387. DOI URL PMID
[51]	K.D. LaCourse, S.B. Peterson, H.D. Kulasekara, M.C. Radey, J. Kim, J.D. Mougous, Nat. Microbiol. 3 (2018) 440-446. DOI URL PMID
[52]	W. Hu, C. Li, J. Dai, H. Cui, L. Lin, Ind. Crops Prod. 130 (2019) 34-41.
[53]	X.K. Ding, S. Duan, X.J. Ding, R.H. Liu, F.J. Xu, Adv. Funct. Mater. 28 (2018), 1802140.
[54]	K. Kanagamani, P. Muthukrishnan, K. Saravanakumar, K. Shankar, A. Kathiresan, Rare Metals 38 (2019) 277-286.
[55]	X.M. Dai, Q.Q. Guo, Y. Zhao, P. Zhang, T.Q. Zhang, X.G. Zhang, C.X. Li, ACS Appl. Mater. Interfaces 8 (2016) 25798-25807.
[56]	X.L. Ye, X.M. Qin, X.R. Yan, J.K. Guo, L.H. Huang, D.J. Chen, T. Wu, Q.S. Shi, S.Z. Tan, X. Cai, Chem. Eng. J. 304 (2016) 873-881. DOI URL
[57]	V. Alt, T. Bechert, P. Steinrücke, M. Wagener, P. Seidel, E. Dingeldein, E. Domann, R. Schnettler, Biomaterials 25 (2004) 4383-4391. DOI URL