Osteogenic and Antibacterial Metal-Polyphenol Drug-Loaded Coating on Biodegradable Zinc for Orthopedic Implants Application

doi:10.11900/0412.1961.2023.00035

Acta Metall Sin

2024, Vol. 60

Issue (11): 1545-1558 DOI: 10.11900/0412.1961.2023.00035

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Osteogenic and Antibacterial Metal-Polyphenol Drug-Loaded Coating on Biodegradable Zinc for Orthopedic Implants Application

LIN Xue¹^,², QIAN Junyu¹^,², ZHANG Wentai¹^,², WANG Peng¹^,², WAN Guojiang¹^,²(

)

1 Key Laboratory of Advanced Technologies of Materials (Ministry of Education), College of Medicine, Southwest Jiaotong University, Chengdu 610031, China
2 School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China

Cite this article:

LIN Xue, QIAN Junyu, ZHANG Wentai, WANG Peng, WAN Guojiang. Osteogenic and Antibacterial Metal-Polyphenol Drug-Loaded Coating on Biodegradable Zinc for Orthopedic Implants Application. Acta Metall Sin, 2024, 60(11): 1545-1558.

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Abstract

Biodegradable metallic Zn materials are being considered for orthopedic implant applications because of their moderate degradation rate and potential bio-functionalities. Nevertheless, their clinical use is limited due to inadequate osteogenic properties owing to Zn²⁺ burst release, premature mechanical failure caused by non-uniform corrosion, and poor antibacterial ability. Therefore, to overcome these issues, a metal-polyphenol drug-loaded coating was functionalized on the surface using an alternating chemical deposition method out of tannic acid/metformin molecules and active metallic ions via coordination/chelation reactions. The coating was characterized by homogeneous compactness, which enhanced the corrosion resistance of the Zn substrate, adjusted the corrosion mode, suppressed the release of Zn²⁺, and regulated metformin release. The in vitro pre-osteoblasts (MC3T3-E1) culture results showed that the coated Zn samples exhibited excellent osteogenic ability. The antibacterial assays with coated Zn samples demonstrated strong antibacterial efficiency.

Key words: biodegradable Zn active metallic ion metal-polyphenol drug-loaded coating osteogenesis antibacterial property

Received: 02 February 2023

ZTFLH:

TG146.1

Fund: National Key Research and Development Program of China(2016YFC1102500);Science and Tech-nology Program of Sichuan Province(2020YFH0077);Science and Tech-nology Program of Sichuan Province(2024YFHZ0310);Open Fund Project of Sichuan Provincial Key Laboratory for Material Corrosion and Protection(2022CL07)

Corresponding Authors: WAN Guojiang, professor, Tel: (028)87600723, E-mail: guojiang.wan@home.swjtu.edu.cn

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	LIN Xue
	QIAN Junyu
	ZHANG Wentai
	WANG Peng
	WAN Guojiang

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https://www.ams.org.cn/EN/10.11900/0412.1961.2023.00035 OR https://www.ams.org.cn/EN/Y2024/V60/I11/1545

Fig.1 Surface SEM images of Zn (a), polyphenol drug-loaded coating (TA/Met) (b), and metal-polyphenol drug-loaded coatings including Cu-TA/Met (c), Fe-TA/Met (d), Mg-TA/Met (e), and Sr-TA/Met (f) (Insets show the high magnified images)

Fig.2 FTIR spectra of Zn, TA/Met, Cu-TA/Met, Fe-TA/Met, Mg-TA/Met, and Sr-TA/Met

Fig.3 High-resolution XPS of C1s (a), N1s (b), O1s (c), Zn2p (d), Cu2p, Fe2p, Mg2p, and Sr3d (e) of TA/Met, Cu-TA/Met, Fe-TA/Met, Mg-TA/Met, and Sr-TA/Met

Table 1 Elements compositions of sample surface according to XPS

Fig.4 Potentiodynamic polarization curves (a), the obtained self corrosion potential (E_corr) and self corrosion current density (i_corr) (b), Nyquist plots and equivalent electrical circuit (inset) (c), Bode-impedance and Bode-phase angle (d) diagrams of the Zn, TA/Met, Cu-TA/Met, Fe-TA/Met, Mg-TA/Met, and Sr-TA/Met in Hank's solution at (37 ± 0.5)^oC (i—gal-vanic current density, Z″—imaginary part of impedance, Z′—real part of impedance, |Z|—impedance modulus, R_s—resistance of electrolyte, Q_p—capacitance of the corrosion products layer, R_p—resistance of the coating, Q_ct—double-layer capacitance, R_ct—resistance of the interfacial charge transfer reaction)

Table 2 Fitting EIS results of samples

Fig.5 Surface SEM images of Zn (a), TA/Met (b), Cu-TA/Met (c), Fe-TA/Met (d), Mg-TA/Met (e), and Sr-TA/Met (f) immersed in Hank's solution at (37 ± 0.5)^oC for 21 d (Insets show the high magnified images)

Fig.6 XRD spectra (a), the accumulated Zn²⁺ concentrations (b), pH value changed with immersion time (c), and metformin concentration (d) of Zn, TA/Met, Cu-TA/Met, Fe-TA/Met, Mg-TA/Met, and Sr-TA/Met immersed in Hank's solution at (37 ± 0.5)^oC for 21 d

Fig.7 Surface SEM images of Zn (a), TA/Met (b), Cu-TA/Met (c), Fe-TA/Met (d), Mg-TA/Met (e), and Sr-TA/Met (f) immersed in Hank's solution at (37 ± 0.5)^oC for 21 d after removal of corrosion products (Insets show the high magnified images)

Fig.8 Fluorescence microscopy images of MC3T3-E1 cultured on stainless steel (SS) (a), Zn (b), TA/Met (c), Cu-TA/Met (d), Fe-TA/Met (e), Mg-TA/Met (f), and Sr-TA/Met (g) for 1 d

Fig.9 Adherent cell amounts (a) and quantification of alkaline phosphatase (ALP) activities (b) of MC3T3-E1 cultured on SS, Zn, TA/Met, Cu-TA/Met, Fe-TA/Met, Mg-TA/Met, and Sr-TA/Met for 1 d (Null hypothesis value of p < 0.05 was labeled as *, p < 0.01 as **, and p < 0.001 as ***)

Fig.10 ALP staining images of MC3T3-E1 cultured on SS (a), Zn (b), TA/Met (c), Cu-TA/Met (d), Fe-TA/Met (e), Mg-TA/Met (f), and Sr-TA/Met (g) for 14 d

Fig.11 Photos of colony numbers (a1-a7, b1-b7) and antibacterial rates (c, d) of S.aureus (a1-a7, c) and E.coli (b1-b7, d) cultured on SS (a1, b1), Zn (a2, b2), TA/Met (a3, b3), Cu-TA/Met (a4, b4), Fe-TA/Met (a5, b5), Mg-TA/Met (a6, b6), and Sr-TA/Met (a7, b7) for 1 d

Fig.12 Schematic of the formation mechanism of metal-polyphenol drug-loaded coating

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