Abstract
An active wound dressing that is biomechanically and biochemically effective is essential for wound care and skin tissue regeneration. Despite its importance, issues persist with mechanical compatibility and drug release control, restricting the optimal use of existing dressings. In this work, we present a simple approach using a poly (vinylidene fluoride) (PVDF) substrate containing zeolitic imidazolate framework (ZIF-8) seeds of different sizes to start the precise development of a highly flexible metal-organic framework membrane with a consistent honeycomb structure, suitable for drug loading and release. With the embedded seeds serving as a control center, the honeycomb membrane formed features pore openings ranging from 0.7 to 3 µm. These adjustable microscale pores, combined with the intrinsic nanopores in ZIF-8, facilitate efficient loading of the anti-inflammatory drug curcumin (CCM) and enable its rapid and controlled release for antibacterial activity and cell growth. Among these, the 0.7-µm honeycomb membrane produced on the 40-nm seed showed a 2-fold increase in cell proliferation compared with the honeycomb membrane (equal to the bare PVDF substrate). Furthermore, it displayed 5 and 2.4 times greater antibacterial activity against Staphylococcus aureus and Escherichia coli than the substrate. These results are attributable to the balanced influence of CCM and Zn2+ release properties from such ideal pore geometries. The controllable and hierarchical pore-arrayed membrane boasts unique characteristics that make it a promising option for wound healing. Additionally, it offers valuable insights for the design of future biomedicine applications.
摘要
具有生物力学和生化活性的敷料在伤口护理和皮肤组织再生中 起着至关重要的作用. 然而, 机械失配和药物释放管理所涉及的问题限 制了当前敷料的有效使用. 在本工作中, 我们报道了一种简单的策略, 即采用聚偏二氟乙烯(PVDF)作为底物, 通过嵌入不同尺寸的沸石咪唑 酸盐框架(ZIF-8)种子, 以推动具有均匀蜂窝结构的高柔性金属有机框 架(MOF)复合膜的受控生长, 用于药物负载和释放. 以嵌入的种子为控 制中心, 形成的多孔膜具有约0.7–3µm的宽孔隙. 这种可调节的微尺度 孔与ZIF-8中的固有纳米孔不仅可以有效地提高抗炎类药物的负载(姜 黄素, CCM), 而且还能够快速并可控地释放药物, 大大提高了抗菌活 性, 同时促进细胞生长. 其中, 在40 nm 种子上生长的0.7 µm 多孔膜的 表现优于其他蜂窝膜, 与2 µm 多孔膜(相当于裸PVDF 基质)相比, 细 胞增殖能力提高了约2倍, 针对金黄色葡萄球菌(S. aureus)和大肠杆菌 (E. coli)的抗菌活性分别提高了5倍和2.4倍, 是基底抗菌活性的5倍, 这 是因为这种最佳孔几何结构具有CCM 和Zn2+ 释放特性的平衡效应. 这种可控分层孔阵列膜的独特性质有望真正用于伤口愈合, 同时也为 生物医学设计提供了新的指导.
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References
Chen G, Wang F, Zhang X, et al. Living microecological hydrogels for wound healing. Sci Adv, 2023, 9: 3478
Nishikawa T, Yamane H, Matsuhisa N, et al. Stretchable strain sensor with small but sufficient adhesion to skin. Sensors, 2023, 23: 1774
Yao J, Sun L, Xiao Y, et al. Impact of surface free energy on two-dimensional crystallization. Sci China Mater, 2023, 66: 1511–1517
Patil P, Russo KA, McCune JT, et al. Reactive oxygen species-degradable polythioketal urethane foam dressings to promote porcine skin wound repair. Sci Transl Med, 2022, 14: 6586
Guo Z, Zhang Z, Zhang N, et al. A Mg2+/polydopamine composite hydrogel for the acceleration of infected wound healing. Bioactive Mater, 2022, 15: 203–213
Yang D, Tian G, Liang C, et al. Double-microcrack coupling stretchable neural electrode for electrophysiological communication. Adv Funct Mater, 2023, 33: 2300412
Zeng L, Liu B, Gao G. Physically crosslinked polyvinyl alcohol/chitosan-phytic acid hydrogels for wearable sensors with highly conductive, recyclable and antibacterial properties. Sci China Mater, 2023, 66: 4062–4070
Wang L, Sun L, Gu Z, et al. N-carboxymethyl chitosan/sodium alginate composite hydrogel loading plasmid DNA as a promising gene activated matrix for in-situ burn wound treatment. Bioact Mater, 2022, 15: 330–342
Zhang X, Xiao L, Ding Z, et al. Engineered tough silk hydrogels through assembling β-sheet rich nanofibers based on a solvent replacement strategy. ACS Nano, 2022, 16: 10209–10218
Qi D, Zhang K, Tian G, et al. Stretchable electronics based on PDMS substrates. Adv Mater, 2021, 33: 2003155
Dong J, Gong Z, Chen Y, et al. Organic microstructure-induced hierarchically porous g-C3N4 photocatalyst. Sci China Mater, 2023, 66: 3176–3188
Thum MD, Lu Q, Stockmaster KT, et al. 3D-printable cyclic peptide loaded microporous polymers for antimicrobial wound dressing materials. Polyms Adv Techs, 2023, 34: 1008–1018
Wang P, Pu Y, Ren Y, et al. Bio-inspired hydrogel-based bandage with robust adhesive and antibacterial abilities for skin closure. Sci China Mater, 2022, 65: 246–254
Mehteroğlu E, Çakmen AB, Aksoy B, et al. Preparation of hybrid PU/PCL fibers from steviol glycosides via electrospinning as a potential wound dressing materials. J Appl Polym Sci, 2020, 137: 49217
Li SF, Chen Y, Wang YS, et al. Integration of enzyme immobilization and biomimetic catalysis in hierarchically porous metal-organic frameworks for multi-enzymatic cascade reactions. Sci China Chem, 2022, 65: 1122–1128
Zhu Y, Xu Z, Wu F, et al. Liquid-crystal elastomers based on covalent adaptable networks: From molecular design to applications. Sci China Mater, 2023, 66: 3004–3021
Chen X, Shuai D, Yang H, et al. Polyoxometalates as potential next-generation metallodrugs in the melanogenesis inhibitor. Z anorg allge Chem, 2022, 648: e202100319
Hang C, Wei Z, Jieyu X, et al. ZIF-8/curcumin-loaded electrospun nanofiber membrane for wound healing. ACS Appl Nano Mater, 2023, 6: 15620–15631
Zhang Q, Cao P-, Cheng Y, et al. Nonlinear ion transport through ultrathin metal–organic framework nanosheet. Adv Funct Mater, 2020, 30: 2004854
Lim JYC, Goh L, Otake K, et al. Biomedically-relevant metal organic framework-hydrogel composites. BioMater Sci, 2023, 11: 2661–2677
Wei TH, Wu SH, Huang YD, et al. Rapid mechanochemical encapsulation of biocatalysts into robust metal–organic frameworks. Nat Commun, 2019, 10: 5002
Chai H, Ma Y, Yuan Z, et al. A ratiometric fluorescence sensor based on carbon dots and two-dimensional porphyrinic MOFs for on-site monitoring of sulfide. MicroChem J, 2023, 185: 108288
Yao MS, Otake K, Xue ZQ, et al. Concluding remarks: current and next generation MOFs. Faraday Discuss, 2021, 231: 397–417
Zou D, Lee YM. Design strategy of poly(vinylidene fluoride) membranes for water treatment. Prog Polym Sci, 2022, 128: 101535
Carraro F, Williams JD, Linares-Moreau M, et al. Continuous-flow synthesis of ZIF-8 biocomposites with tunable particle size. Angew Chem Int Ed, 2020, 59: 8123–8127
Sun Y, Liu Y, Caro J, et al. In-plane epitaxial growth of highly c-oriented NH2-MIL-125(Ti) membranes with superior H2/CO2 selectivity. Angew Chem Int Ed, 2018, 57: 16088–16093
Wu C, Xiong Z, Li C, et al. Zeolitic imidazolate metal organic framework ZIF-8 with ultra-high adsorption capacity bound tetracycline in aqueous solution. RSC Adv, 2015, 5: 82127–82137
Moussawi RN, Patra D. Modification of nanostructured ZnO surfaces with curcumin: fluorescence-based sensing for arsenic and improving arsenic removal by ZnO. RSC Adv, 2016, 6: 17256–17268
Mohamed ME, Abd-El-Nabey BA. Fabrication of a biological metal–organic framework based superhydrophobic textile fabric for efficient oil/water separation. Sci Rep, 2022, 12: 15483
Kang L, Liang Q, Abdul Q, et al. Preparation technology and preservation mechanism of γ-CD-MOFs biaological packaging film loaded with curcumin. Food Chem, 2023, 420: 136142
Morozova AS, Vilchevskaya EN, Müller W, et al. A holistic continuum model-based approach to drug release. Continuum Mech Thermodyn, 2022, 34: 81–91
Wang Y, Ying T, Li J, et al. Hierarchical micro/nanofibrous scaffolds incorporated with curcumin and zinc ion eutectic metal organic frameworks for enhanced diabetic wound healing via anti-oxidant and anti-inflammatory activities. Chem Eng J, 2020, 402: 126273
Petropoulos JH, Papadokostaki KG, Sanopoulou M. Higuchi’s equation and beyond: Overview of the formulation and application of a generalized model of drug release from polymeric matrices. Int J Pharm, 2012, 437: 178–191
Shahed CA, Ahmad F, Gunister E, et al. Antibacterial mechanism with consequent cytotoxicity of different reinforcements in biodegradable magnesium and zinc alloys: A review. J Magnesium Alloys, 2023, 11: 3038–3058
Costello LC, Franklin RB. Cytotoxic/tumor suppressor role of zinc for the treatment of cancer: an enigma and an opportunity. Expert Rev Anticancer Ther, 2012, 12: 121–128
Zhang Y, Chang M, Bao F, et al. Multifunctional Zn doped hollow mesoporous silica/polycaprolactone electrospun membranes with enhanced hair follicle regeneration and antibacterial activity for wound healing. Nanoscale, 2019, 11: 6315–6333
Liu X, You L, Tarafder S, et al. Curcumin-releasing chitosan/aloe membrane for skin regeneration. Chem Eng J, 2019, 359: 1111–1119
Yasayan G, Karaca G, Akgüner ZP, et al. Chitosan/collagen composite films as wound dressings encapsulating allantoin and lidocaine hydrochloride. Int J Polymic Mater Polymic Biomater, 2021, 70: 623–635
Li Z, Wang Q, Mi W, et al. Effects of negative-pressure wound therapy combinedwith microplasma on treating wounds of ulcer and the expression of heat shock protein 90. Exp Therapeutic Med, 2017, 13: 2211–2216
Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (52371248), National Key R&D Program of China (2021YFB3802200), Guangdong Basic and Applied Basic Research Foundation (2023A1515010905) and the Scientific and Technological Innovation Foundation of Shunde Graduate School, USTB (BK22BE012). Lee HK thanks the funding supports from Singapore Ministry of Education (AcRF Tier 1 RS13/20 and RG4/21), A*STAR Singapore (AME YIRG A2084c0158), the Center ofHydrogen Innovation, National University of Singapore (CHI-P2022-05), and Nanyang Technological University Startup Grants.
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Author contributions Li J conducted the experiments, processed the data, and wrote the paper. Fang Q drew some illustrations. Yan Y conceived the work and wrote the paper. Chen Y wrote the paper. Lee HK edited and reviewed paper. Wang LN supervised the project. All the authors contributed to the general discussion. All authors read and agreed to the published version of the manuscript.
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Yingzhi Chen is an associate Professor at the School of Materials Science and Engineering, University of Science and Technology Beijing. She received her PhD degree in chemistry from the Institute of Technical Institute of Physics & Chemistry, Chinese Academy of Sciences in 2012 after she got her MS degree in chemistry from Beijing Normal University. Her current research focuses on the design and synthesis of novel organic semiconductor nanocrystals and their applications in photocatalysis and biosensing.
Lu-Ning Wang is a Professor at the School of Materials Science and Engineering, University of Science and Technology Beijing. He received his BE and MS degrees in materials science and engineering from the University of Science and Technology Beijing, in 2002 and Tsinghua University in 2005, respectively. He received another BE and PhD degrees in medical science and biomedical engineering from the University of Alberta in 2007 and 2011, respectively. His research interests include optoelectronic materials and biodgradable materials.
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Li, J., Yan, Y., Fang, Q. et al. Highly flexible and controllable hierarchical MOF membrane for efficient drug release. Sci. China Mater. 67, 1509–1520 (2024). https://doi.org/10.1007/s40843-024-2909-9
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DOI: https://doi.org/10.1007/s40843-024-2909-9