ZIF-L coated cotton fabric for antibacterial and self-cleaning applications

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Zeolitic imidazolate framework-L (ZIF-L) nanostructures have gained significant attention in research due to their ability to sustainably release Zn 2+ ions, coupled with the physical destruction of bacteria by their blade tips. Integrating natural fabrics with ZIF-L represents an effective approach to enhancing the value-added features of textiles with unique functionalities. In this study, we reported a facile technology for the in-situ growth of ZIF-L on cotton fabrics. A uniform and dense coating of leaf-shaped nanostructures by doping Cu 2+ ions on ZIF-L was formed on the cotton fiber surface (Cu@ZIF-L@Cotton), followed by treatment with methyltrimethoxysilane (MTMS) to obtain water-repellent MTMS/Cu@ZIF-L@Cotton fabric. The resulting fabrics exhibited excellent antibacterial activities against both Gram-negative and Gram-positive bacteria, effectively killing 5 log CFU (>99.999%) of E. coli and S. aureus. Furthermore, the prepared cotton fabric not only showed hydrophobicity with a water contact angle of 132° ± 0.58 but also displayed good self-cleaning properties. Additionally, these fabricated fabrics showed good functional stability after washing. It is therefore believed these valuable functions could significantly enhance the practical feasibility of the fabric in various application scenarios. ZIF-L cotton MTMS antibacterial self-cleaning Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Introduction Bacterial infections pose an increasingly grave threat to public health, and effectively combating these threats on a large scale has become an uphill task (Halloran 2014 ). Transmission via contaminated surfaces has been recognized as a significant pathway for spreading pathogenic microorganisms (Mallakpour et al. 2021 ; Nasri et al. 2021 ). The COVID-19 pandemic has heightened global attention to the transmission of contamination facilitated by high-touch surfaces, for example, textiles, public transport, and so on (Imani et al. 2020a ). In response, relevant researchers are currently investigating the utilization of surfaces and coatings that possess the capability to inhibit the proliferation and dissemination of microorganisms through either eradication or reduction of microbial adhesion to textile surfaces, given that textiles serve as high-contact materials. The achievement of these goals has been facilitated by the utilization of surface-bound active antimicrobials (Qiu et al. 2022 ), as well as the development of biocidal coatings (Ye et al. 2021 ) and passive pathogen-repellent surfaces employing nanomaterials (Imani et al. 2020b ), chemical modifications, and micro- and nanostructuring techniques (Crawford et al. 2012 ; Shen et al. 2021 ). The utilization of metal-organic frameworks (MOFs) nanostructures, exemplified by zeolitic imidazolate frameworks (ZIFs), holds immense potential due to their inherent antibacterial activity, in conjunction with their ability to function as a reservoir for metal ions (Zhuang et al. 2012 ; Taheri et al. 2021 ). ZIF-L, formed by linking zinc ions and the organic ligand 2-methylimidazole (2-MI), exhibits the same structural unit as that of ZIF-8. Both ZIF-L and ZIF-8 possess good antibacterial properties, attributed to the release of Zn 2+ ions and imidazole-like antibacterial organic ligands (Yuan and Zhang 2017 ; He et al. 2023 ; Li et al. 2023 ). Furthermore, the nano-dagger arrays of ZIF-L prevent bacterial growth by rupturing the adhered microbial cells through their sharp tips (Yuan et al. 2019 ). The ZIF-L nano-structure is typically grown in situ on textile surfaces, and constructing the microstructures/nanostructures on the surface of substrates, thereby imparting antibacterial properties to the fabric and simultaneously enhancing its surface roughness. Despite these advances, there are still exit challenges that need to be addressed, particularly concerning the aggregation and poor durability of ZIF-L on textile surfaces. Moreover, the recent emergence of self-cleaning cotton fabrics with antibacterial properties has garnered significant attention. Due to the abundant presence of hydroxyl groups on its surface, cellulose-based fibers exhibit high absorbency and are prone to staining when exposed to liquids(Xu et al. 2010 ). Generally, there are two approaches to fabricating self-cleaning textiles. One approach involves the creation of a photocatalytic fabric with properties such as TiO 2 , which facilitates the decomposition of most stains on the fabric (Karimi and Esmail 2014 ). The other approach focuses on preparing superhydrophobic fabrics that exhibit resistance towards various liquids, enabling easy removal of dirt from the fabric through water. The superhydrophobic surface can be achieved by combining the synergistic effects of low surface energy materials (fluoride, alkane) and rough hierarchical structures (micro-, nano-, or micro/nanostructures) (Wen et al. 2015 ; Li and Guo 2019 ; Li et al. 2022 ). Inspired by these results, we believe that taking advantage of the morphological evolution of ZIF-L to develop the hydrophobic structure is a promising strategy for constructing antibacterial and self-cleaning materials. In this study, we described a convenient approach for fabricating copper ion doping ZIF-L (Cu@ZIF-L) on cotton fabrics via an in-situ growth method. By adjusting the molar ratio of 2-MI/Zn 2+ and reaction time, both the quantity and morphology of ZIF-L could be modulated. Then, treatment with MTMS led to the formation of hydrophobic cotton fabric (MTMS/Cu@ZIF-L@Cotton). The antibacterial activities against E. coli and S. aureus were evaluated, along with investigations into hydrophobicity and self-cleaning properties. Additionally, functional stability after washing was also assessed. Experimental Materials Plain-woven cotton fabrics (120 g/m 2 ) were purchased from Qinzhe Textiles Co., Ltd. 2-methylimidazole (2-MI), zinc chloride (ZnCl 2 ) and Methyltrimethoxysilane (MTMS) were supported from Shanghai Macklin Biochemical Technology Co., Ltd. Copper chloride dihydrate (CuCl 2 ) were purchased from Sinopharm Chemical Reagent Co., Ltd. All chemical reagents were used as received unless specified otherwise. Fabrication of ZIF-L@Cotton The raw cotton fabrics were rinsed in ethanol and deionized (DI) water by sonication for 30 min as pretreated first. After drying, cotton fabrics were cut into 2 cm × 5 cm and put into a ziplock bag for later use. The pretreated cotton fabric was immersed vertically in 200 mL of aqueous solution of 2-MI (0.35 M) for 30 min. After that, 20 mL of ZnCl 2 aqueous solution (0.5 M) was introduced dropwise. After stirring for 3 h, the cotton fabric was taken out, washed with ethanol and DI water, and then dried under vacuum at 65 ℃ to obtain ZIF@Cotton. In addition, other ZIF@Cotton with different molar ratios (2-MI/Zn 2+ = 5:1) and different times (1h, 3h, and 5h) were prepared. The ZIF@Cotton (from 2-MI/Zn 2+ = 7:1, 3 h) was used for further characterization. Fabrication of Cu@ZIF-L@Cotton Cu@ZIF-L@Cotton was prepared as follows: the cotton fabric was placed vertically in the aqueous solution of 2-MI (0.35 M), and then the mixture of ZnCl 2 and CuCl 2 aqueous solution (4 M:1 M) was introduced dropwise to the above solution and kept still for another 3 h. Afterward, the fabric was removed, washed several times with ethanol and DI water, and then dried at 65 ℃ in an oven. Also, other Cu@ZIF@Cotton with different molar ratios (2-MI/Zn 2+ = 5:1) and different times (1h, 3h, and 5h) were prepared. The Cu@ZIF@Cotton (from 2-MI/Zn 2+ = 7:1, 3 h) was used for the following modification. Fabrication of MTMS/Cu@ZIF-L@Cotton The hydrophobic method was followed according to a previous report (Fei et al. 2022 ). The Cu@ZIF-L@Cotton sample and a petri dish containing MTMS were placed in a drying vessel. The drying vessel was sealed and then heated at 70 ℃ for 3 h. After that, unreacted MTMS was removed by placing the modified samples in a vacuum oven at 60 ℃ for 1 h. Hydrophobic cotton fabric (MTMS/Cu@ZIF-L@Cotton) was then achieved. Characterizations The surface morphology and elemental compositions were examined using field emission scanning electron microscope (FE-SEM, Ultra-55, Carl Zesis, Germany) and energy dispersive spectrometer (EDS), respectively. The Fourier transform infrared spectroscopy (FT-IR, Nicolet 5700, Thermo Fisher Scientific, USA) data were collected in the range of 400—4000 cm − 1 . The composition was measured with the X-ray photoelectron spectrometer (XPS, K-ALPHA, Thermo Fisher Scientific, USA). The water contact angle (WCA) of the samples was measured using a Contact Angle Analyzer (JY-PHb, Bingjing, China) at room temperature. Bacterial adhesion test The cotton fabrics, before and after modification, were immersed in 25 mL of bacterial suspension ( S. aureus ) containing 10 7 CFU mL − 1 and incubated under static conditions at 37 ℃ for 2 h. Subsequently, the fabrics were taken out and held vertically for 3 min to allow any remaining droplets to slide away. Following this, the fabrics were washed twice with 5 mL of sterile water to remove any unadhered bacteria. Next, the cotton fabrics were fixed with 2.5% glutaraldehyde solution for 2 h at 4 ℃ and then rinsed twice with PBS. Afterward, the samples were dehydrated using a series of graded ethanol solutions (50, 75, 90, and 100 wt %, for 15 min each) and then observed under SEM after drying and treatment with platinum. Antibacterial test Gram-negative Escherichia coli ( E. coli ) and Gram-positive Staphylococcus aureus ( S. aureus ) were chosen for the antibacterial activity assessment by the zone of inhibition (ZOI) and shaking flask plate method. The cotton fabrics were cut into circular samples with a radius of 1 cm. A 200 µL of bacterial suspension (10 5 CFU/mL) was plated onto the LB agar plates. The cotton fabrics were placed on the surface of the LB agar and incubated at 37 ℃ for 24 h. The pristine cotton fabric was used as control. The shaking flask plate method was performed as follows, bacteria were diluted to approximately ~ 10 5 CFU mL − 1 in PBS (70 mL). The cotton fabric samples (0.75 ± 0.05 g) were cut into pieces and added to the bacterial suspension, which was incubated at 37 ℃ for 24 h with shaking at 130 rpm. After that, 100 µL of culture medium was removed and serially diluted to the appropriate dilution before plating onto LB agar plates. The bacteria were incubated at 37 ℃ for 24 h. After that, the number of bacterial colonies on the plates was counted and the killing rate was evaluated using the following equation: $$\:Antibacterial\:Rate=({C}_{control}-{T}_{sample})/{C}_{control}\times\:100$$ where \(\:{C}_{control}\) is the number of bacterial colonies of the control sample; \(\:{T}_{sample}\) is the number of bacterial colonies of the treated cotton fabrics. Results and discussion In this study, a hydrophobic antibacterial cotton fabric was achieved via a simple in-situ deposition method, as shown in Scheme 1 . First, the cotton fabric was vertically immersed in a precursor solution containing 2-MI. Upon the addition of ZnCl 2 or ZnCl 2 /CuCl 2 , simultaneous nucleation and crystal growth took place on the cotton fabrics. Alternatively, Cu 2+ could form coordination with dimethylimidazole; however, its binding affinity was comparatively weaker than that of Zn 2+ (Yang et al. 2023 ). During this process, ZIF-L or Cu@ZIF-L formed and deposited on the fabric surface, which could be attributed to electrostatic and coordination interaction between the hydroxyl groups of cellulose and Zn 2+ /Cu 2+ ions (Yang et al. 2020 ). The Cu@ZIF-L@Cotton fabric was subsequently subjected to chemical vapor deposition of MTMS for surface modification, aiming to achieve a low-energy state and thereby obtain a hydrophobic cotton fabric. The surface morphology structure of the pristine and modified cotton fabrics was characterized by SEM. As shown in Figure S1 , the pristine cotton fabric has a smooth surface. When ZIF-L or Cu@ZIF-L were formed and in-suit grew on the surface of cotton fabric, the surface morphology of cotton fibers was changed obviously. As shown in Figs. 1 a and b, the coated cotton fabric was covered by a thick layer of ZIF-L or Cu@ZIF-L nano-dagger. Each nano-dagger resembled a vertically extending sharp-tipped leaf, intricately arranged on the cotton fabric surface and fully covered the substrates. These structures correspond to the characteristic appearance of the ZIF-L nanostructure. The observed vertical alignment could primarily be attributed to the confined growth of ZIF-L, wherein the complete coverage of cotton fiber by small ZIF-L crystals leads to the subsequent appearance of larger ZIF-L crystals during continuous growth. As indicated by the red arrows, the ZIF scattered on the fabric surface reveals nano-dagger with dimensions of ~ 2 µm in width and ~ 6 µm in height. By adjusting the molar ratio of 2-MI/Zn 2+ and reaction time, the amount and morphology of the ZIF-L could be changed (Figure S2 ). When the amount of 2-MI was low, the surface coverage of the fabric appeared incomplete or the structure of the surface layer was indistinct. With an increase in the content of 2-MI and reaction time, both the size and density of ZIF-L or Cu@ZIF-L exhibit a corresponding increase. Notably, as shown in Figure S3, for Cu@ZIF-L, at a molar ratio of 2-MI to Zn 2+ equal to 5, a relatively sparse distribution of Cu@ZIF-L was observed on the fabric surface. When the ratio of 2-MI to Zn 2+ reached 7:1, the dense and uniform layer of Cu@ZIF-L be achieved. After MTMS modification, it could be observed that the morphological structure is unchanged compared with Cu@ZIF-L@Cotton fabric, and it was still coated with a tight nano-dagger structure (Fig. 1 c). The chemical composition of samples was characterized using EDS mapping. In the case of ZIF@Cotton, C, O, N, and Zn elements were detected (Figure S4a). Additionally, Cu element was observed in Cu@ZIF@Cotton along with the aforementioned elements found in ZIF@Cotton (Figure S4b). These results further confirmed the successful formation of ZIF-L or Cu@ZIF-L on the surface of cotton fibers. Furthermore, EDS analysis revealed that MTMS/Cu@ZIF-L@Cotton exhibited surface elements including C, O, N, Zn, Cu, and Si (from MTMS) (Fig. 1 d). Notably, these elements were uniformly distributed on the surface of fabric fibers, so it could be proved that MTMS was well attached to the surface of the Cu@ZIF-L@Cotton. The chemical composition of different samples was characterized by FT-IR, which was depicted in Figs. 2 a and b. For ZIF-L and Cu@ZIF-L, the absorption peak at 3100 cm − 1 and 2920 cm − 1 belonged to the aromatic and aliphatic C-H stretch of imidazole, respectively. The peak observed at 1147 cm − 1 corresponded to the C-N stretching vibration of imidazole linkers in ZIF-L. The strong absorption bands detected at 757 cm − 1 and 690 cm − 1 could be attributed to the out-of-plane bending of the Hmim ring, while the band observed at 1308 cm − 1 was associated with the in-plane bending (Zhang et al. 2018 ). The band observed at 1567 cm − 1 corresponded to the C = N double band stretching vibration. Furthermore, the absorption peak around 420 cm − 1 signified the Zn-N stretching mode of the formed ZIF-L, indicating the coordination of Zn 2+ with nitrogen atoms in 2-MI to form imidazolate(Bustamante et al. 2014 ). The absorption peak at about 550–620 cm − 1 belonged to the Cu-N bond, which was observed on the spectrum of Cu@ZIF-L (Yang et al. 2023 ). This suggested the successful embedding of Cu 2+ on ZIF-L. As depicted in Fig. 2 b, the pristine cotton fabric exhibited only two main characteristic peaks at 2901 cm − 1 and 3320 cm − 1 , corresponding to the stretching vibrations of C-H and -OH groups, respectively. After the deposition of ZIF-L and Cu@ZIF-L, distinct characteristic peaks attributed to ZIF-L and Cu@ZIF-L emerged, indicating the successful growth of these materials on the cotton substrate. After the silane modification, the MTMS/Cu@ZIF-L@Cotton exhibited two new characteristic peaks at 1262 cm − 1 and 801 cm − 1 , attributed to Si-CH 3 and Si-O-Si, indicating the formation of a siloxane network (Qin et al. 2021 ; Fan et al. 2023 ). To further determine the chemical composition changes of fabrics at each modification step, the XPS testing was performed to further study the elemental composition and valence of the related samples. In the wide-scan XPS spectrum of pristine cotton fabric, as shown in Fig. 2 c, only peaks corresponding to C1s and O1s were observed. Upon deposition of ZIF-L, three additional peaks emerged at 1044.58 eV, 1021.62 eV, and 400.09 eV, which could be attributed to Zn 2p 1/2, Zn 2p 3/2, and N1s states respectively (Fig. 2 d) (Ananth et al. 2017 ; Wang et al. 2023 ). After depositing Cu@ZIF-L, resulted in the appearance of Cu 2p peaks in addition to the aforementioned ones. The high-resolution spectrum of Cu 2p was divided into three parts (Fig. 2 e), in which the peaks centered at approximately 953.18 and 933.35 eV correspond to Cu 2p 1/2 and Cu 2p 3/2, respectively (Li et al. 2019 ). Additionally, it is noteworthy that two satellite peaks were observed at 944.48 and 940.82 eV, indicating the predominant presence of the Cu 2+ valence state (Elfeky et al. 2019 ; Sun et al. 2020 ). In addition, the deconvolution of N 1s revealed three distinct peaks at 407.50, 400.08, and 398.75 eV (Fig. 2 f), corresponding to the N = C, N − Zn & N − Cu, and N − C bonds respectively (Bhattacharyya et al. 2016 ; Yang et al. 2023 ). Furthermore, after coating with MTMS, two new peaks around 101.0 (Si 2p) and 154.4 (Si 2s), indicating that Cu@ZIF-L@Cotton fabric was covered by MTMS (Yang et al. 2021 ). The wettability of a material's surface is comprehensively determined by its chemical composition, surface roughness, and surface energy(Campoccia et al. 2013 ). Measurement of the water contact angle (WCA) is widely employed to characterize the surface wettability of materials. The WCA of the original cotton fabric was 0°, indicating a good hydrophilic (Fig. 3 a). After surface modification by in-situ grown ZIF-L or Cu@ZIF-L, the WCA of the ZIF-L@Cotton and Cu@ZIF-L@Cotton fabric was still 0° on the basis of the increased surface roughness (Figs. 3 b and c). The subsequent modification of MTMS on the Cu@ZIF-L@Cotton enhanced the hydrophobicity with a WCA of 132° ± 0.58 (Fig. 3 d). The synergy between nanostructures and low surface energy contributes to the good hydrophobic performance of this material. In addition, water droplets repel the fabric surface when the contact angle is tested, which also illustrates the hydrophobicity of the sample surface (Fig. 3 e and Movie S1). Furthermore, as shown in Fig. 3 f, four kinds of droplets including dyed red water, milk, coffee, and juice steadily stood on the surface of Cu@ZIF-L@Cotton fabric displaying good anticontamination and water-resistant properties. To investigate the self-cleaning capability of the as-prepared fabric, the surface of Cu@ZIF-L@Cotton was contaminated with Congo red dye powders. As shown in Fig. 3 g, water droplets could roll easily away from the surface carrying away the Congo red dye from the fabric surface. Therefore, the as-prepared Cu@ZIF-L@Cotton fabric showed good self-cleaning performance. Furthermore, Gram-positive S. aureus was selected as the representative microorganism to explore the bacterial repellency properties. The adherence of bacteria on cotton, Cu@ZIF-L@Cotton, and MTMS/Cu@ZIF-L@Cotton fabrics was observed by SEM as shown in Fig. 3 h. For cotton fabric, large amounts of bacteria adhere to the raw cotton fabric surface. Cu@ZIF-L@Cotton fabric also exhibited a significant adherence of S. aureus to the Cu@ZIF-L nanostructures. On one hand, the positive electrical property of Cu@ZIF-L enabled it to attract negatively charged bacteria. On the other hand, owing to its metal ion core and unsaturated nitrogen from the organic linker, Cu@ZIF-L exhibited an affinity for amino acid residues (Tanum et al. 2022 ), which are abundant in peptidoglycan-the main component of S. aureus cell wall (Romaniuk and Cegelski 2015 ) (Nikolic and Mudgil 2023 )-thus facilitating its attraction towards bacteria. While in the MTMS/Cu@ZIF-L@Cotton fabric, the adhered bacteria were reduced. The hydrophobicity surface demonstrated the repelling effect against bacteria, those tenacious bacteria that managed to be in touch with the surface were killed by Cu@ZIF-L itself. The antibacterial performance of as-prepared Cu@ZIF-L@Cotton fabric was evaluated using the agar diffusion plate method and shake flask method against E. coli and S. aureus . As displayed in Fig. 4 a and Table 1 , without inhibition zone around the pristine cotton was observed for E. coli and S. aureus . For ZIF-L@Cotton and Cu@ZIF-L@Cotton fabric, obvious inhibition zones were seen against all of the strains compared to the uncoated sample fabric. However, after MTMS coating, the distinct inhibition zone was still observed except for a slight decrease against E. coli and S. aureus , which might be attributed to the prohibition of the diffusion of Zn 2+ and Cu 2+ by hydrophobic treatment. The shaking flask method was also employed to assess their antibacterial activities. As depicted in Fig. 4 b, the ZIF-L@Cotton, and Cu@ZIF-L@Cotton fabrics exhibited pronounced antibacterial properties compared to the pristine cotton fabric. The antibacterial efficacy of the ZIF-L@Cotton fabric against S. aureus was significantly superior to that against E. coli , owing to the absence of an outer membrane in Gram-positive bacteria ( S. aureus ), rendering them more susceptible to destruction as opposed to Gram-negative bacteria ( E. coli ) with their dual-membrane structure separated by peptidoglycan (Han et al. 2018 ). Remarkably, the Cu@ZIF-L@Cotton fabric demonstrated exceptional antibacterial activities, achieving a 5 log CFU reduction of both E. coli and S. aureus , indicating a promising killing efficacy of 99.999%. Consequently, doping Cu 2+ into ZIF-L enhanced the antibacterial properties of the fabric considerably. Furthermore, it was worth noting that the antibacterial properties of the sample remained unaffected by modification through MTMS, as evidenced by the absence of bacterial growth on the agar plate. The MTMS/Cu@ZIF-L@Cotton fabric exhibited remarkable antibacterial properties and self-cleaning capabilities, effectively killing tenaciously adhered bacteria on its surface due to the exceptional antibacterial efficacy of Cu@ZIF-L. Table 1 Zone of inhibition (mm) of samples. Microorganism Pristine Cotton ZIF-L@Cotton Cu@ZIF-L@Cotton MTMS/Cu@ZIF-L@Cotton E. coli /mm 0 10.2 10.3 5.8 S. aureus /mm 0 11.2 12.9 8.8 The functional stability of the as-prepared cotton fabric against washing was evaluated by testing the changes in the inhibition zone and WCA. As shown in Fig. 5 a, the Cu@ZIF-L@Cotton fabric still displayed an obvious inhibition zone after undergoing washing, indicating its good antibacterial activity. In addition, the WCA of the Cu@ZIF-L@Cotton fabric was still above 120° after undergoing five laundering cycles. These results indicated that the cotton fabric prepared in this study exhibited good functional stability. Conclusion In summary, antibacterial and self-cleaning properties were imparted to cotton fabrics by in-situ growth of Cu@ZIF-L nanostructures on their surface, followed by modification using MTMS via chemical vapor deposition (MTMS/Cu@ZIF-L@Cotton). Dagger-like ZIF-L nanostructures were vertically grown on the cotton surface, effectively addressing agglomeration issues. The incorporation of Cu 2+ ions enhanced the antibacterial efficacy, demonstrating remarkable antimicrobial activity against E. coli and S. aureus by achieving 5-log of CFU reduction for both bacterial strains. Moreover, the prepared cotton fabric exhibited hydrophobicity and excellent self-cleaning properties. Additionally, these fabricated fabrics demonstrated good functional stability even after 5 washing cycles. The obtained positive outcomes indicate that the developed cotton fabric exhibits great potential as a promising candidate for various applications in the biomedical field. Declarations Funding We acknowledge financial support from the Zhejiang Provincial Natural Science Foundation of China (Grant No. LQ23E030012); and the Scientific Research Foundation of Zhejiang Sci-Tech University (Grant No. 22202001-Y). Author contributions Qiaohua Qiu: Conceptualization; Methodology; Data curation; Writing. LiYing Lan: Material preparation; Data collection. Data availability Data can be available from the corresponding author ( [email protected] ) upon academic reasonable request. Conflict of interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. 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ACS Appl Mater Interfaces 13:14653–14661. https://doi.org/10.1021/acsami.0c22090 Sun S, Yang Z, Cao J, et al (2020) Copper-doped ZIF-8 with high adsorption performance for removal of tetracycline from aqueous solution. J Solid State Chem 285:121219. https://doi.org/10.1016/j.jssc.2020.121219 Taheri M, Ashok D, Sen T, et al (2021) Stability of ZIF-8 nanopowders in bacterial culture media and its implication for antibacterial properties. Chem Eng J 413:127511. https://doi.org/10.1016/j.cej.2020.127511 Tanum J, Choi M, Jeong H, et al (2022) Generation of zinc ion-rich surface via in situ growth of ZIF-8 particle: Microorganism immobilization onto fabric surface for prohibit hospital-acquired infection. Chem Eng J 446:137054. https://doi.org/10.1016/j.cej.2022.137054 Wang L, Wang J, Tang M, et al (2023) Developing a Z-scheme Ag2CO3/ZIF-8 heterojunction for the surface decoration of cotton fabric toward repeatable photocatalytic dye degradation. Appl Surf Sci 610:155605. https://doi.org/10.1016/j.apsusc.2022.155605 Wen L, Tian Y, Jiang L (2015) Bioinspired super-wettability from fundamental research to practical applications. Angew Chemie - Int Ed 54:3387–3399. https://doi.org/10.1002/anie.201409911 Xu B, Cai Z, Wang W, Ge F (2010) Preparation of superhydrophobic cotton fabrics based on SiO2 nanoparticles and ZnO nanorod arrays with subsequent hydrophobic modification. Surf Coatings Technol 204:1556–1561. https://doi.org/10.1016/j.surfcoat.2009.09.086 Yang W, Li L, Chen M, et al (2023) Sustained Endogenous Nitric Oxide Catalytic System Endows Skin Scaffolds with Antibiofilm and Antibacterial Activities. ACS Appl Polym Mater. https://doi.org/10.1021/acsapm.3c01583 Yang Y, Guo Z, Huang W, et al (2020) Fabrication of multifunctional textiles with durable antibacterial property and efficient oil-water separation via in situ growth of zeolitic imidazolate framework-8 (ZIF-8) on cotton fabric. Appl Surf Sci 503:144079. https://doi.org/10.1016/j.apsusc.2019.144079 Yang Y, Zhang S, Huang W, et al (2021) Multi-functional cotton textiles design using in situ generating zeolitic imidazolate framework-67 (ZIF-67) for effective UV resistance, antibacterial activity, and self-cleaning. Cellulose 28:5923–5935. https://doi.org/10.1007/s10570-021-03840-8 Ye Z, Li S, Zhao S, et al (2021) Textile coatings configured by double-nanoparticles to optimally couple superhydrophobic and antibacterial properties. Chem Eng J 420:127680. https://doi.org/10.1016/j.cej.2020.127680 Yuan Y, Wu H, Lu H, et al (2019) ZIF nano-dagger coated gauze for antibiotic-free wound dressing. Chem Commun 699–702. https://doi.org/10.1039/c8cc08568d Yuan Y, Zhang Y (2017) Enhanced biomimic bactericidal surfaces by coating with positively-charged ZIF nano-dagger arrays. Nanomedicine Nanotechnology, Biol Med 13:2199–2207. https://doi.org/10.1016/j.nano.2017.06.003 Zhang S, Du M, Shao P, et al (2018) Carbonic Anhydrase Enzyme-MOFs Composite with a Superior Catalytic Performance to Promote CO2 Absorption into Tertiary Amine Solution. Environ Sci Technol 52:12708–12716. https://doi.org/10.1021/acs.est.8b04671 Zhuang W, Yuan D, Li JR, et al (2012) Highly potent bactericidal activity of porous metal-organic frameworks. Adv Healthc Mater 1:225–238. https://doi.org/10.1002/adhm.201100043 Scheme Scheme 1 is available in the Supplementary Files section. Additional Declarations No competing interests reported. Supplementary Files MovieS1.mp4 SupportingInformation.docx floatimage1.png Scheme 1. Fabrication scheme of MTMS/Cu@ZIF@Cotton fabrics. Cite Share Download PDF Status: Published Journal Publication published 24 Jan, 2025 Read the published version in Cellulose → Version 1 posted Editorial decision: Revision requested 01 Sep, 2024 Editor assigned by journal 31 Aug, 2024 Submission checks completed at journal 31 Aug, 2024 First submitted to journal 26 Aug, 2024 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4975082","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":348028614,"identity":"fd8ed779-8baa-4289-a90e-8aba2ba46671","order_by":0,"name":"Qiaohua Qiu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAuUlEQVRIiWNgGAWjYFACxgYQYuBnZj78gDQtku1saQYkWcRgcJ5HQYIo1XzHkxs/fNxxWN74MA+DAUONTTRBLZJnHjZLzjxz2HDbYd4DDxiOpeU2ENJicCOxQZq37TDjtsN8CQaMDYeJ0tL8G6jFfnMzj4EEsVraQLYkbmAmVgvQL22WM9vSk2ccBgZyAjF+4Tue/vjGxzZr2/7+w4cffKixIayF4UACEicBhyI8WkbBKBgFo2AUYAMAjkpFgDRYV7cAAAAASUVORK5CYII=","orcid":"","institution":"Zhejiang Sci-Tech University","correspondingAuthor":true,"prefix":"","firstName":"Qiaohua","middleName":"","lastName":"Qiu","suffix":""},{"id":348028616,"identity":"ebaf2157-e799-4e76-8921-0155d75e2a7b","order_by":1,"name":"Liying Lan","email":"","orcid":"","institution":"Zhejiang Sci-Tech University","correspondingAuthor":false,"prefix":"","firstName":"Liying","middleName":"","lastName":"Lan","suffix":""}],"badges":[],"createdAt":"2024-08-26 04:02:27","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4975082/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4975082/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s10570-025-06400-6","type":"published","date":"2025-01-24T15:57:06+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":65682182,"identity":"de745b0d-aabf-4188-be27-b8fdf678bd45","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":1102974,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Low- and high-magnification images of ZIF-L@Cotton fabric. (b) Low- and high-magnification images of Cu@ZIF-L@Cotton fabric. (c) Low- and high-magnification images of MTMS/Cu@ZIF-L@Cotton fabric. (d) EDS mapping analysis showing the element distribution in MTMS/Cu@ZIF@Cotton.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/83ac8e0382c9907d8684f520.png"},{"id":65682177,"identity":"abaeafeb-0e09-4c12-9f8a-9adb4f9a7f9a","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":269596,"visible":true,"origin":"","legend":"\u003cp\u003e(a-b) FTIR spectra of related samples. (c) XPS spectrum of related samples. (d-f) Deconvolution of XPS spectra of Zn 2p, Cu 2p, and N 1s.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/b2d65c05a0680f82849d33cc.png"},{"id":65682178,"identity":"bf43435f-81d4-487f-8a57-c5a848beda81","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":376485,"visible":true,"origin":"","legend":"\u003cp\u003eStatic WCA measurement on (a) raw cotton fabric, (b) ZIF-L@Cotton, (c) Cu@ZIF-L@Cotton,and (d) MTMS/Cu@ZIF-L@Cotton. (e) Water droplets repel the fabric surface when the contact angle is tested. (f) The steady state of four kinds of droplets including dyed red water, milk, coffee, and juice on the surface of the fabric. (g) Self-cleaning evaluation of the Cu@ZIF-L@Cotton fabric (Congo red dye was used as a model of contamination). (h) The adherence of bacteria on cotton, Cu@ZIF-L@Cotton, and MTMS/Cu@ZIF-L@Cotton fabrics.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/7d2abc7661fd59bae9cd9b89.png"},{"id":65682179,"identity":"881bc8e4-bc03-49cc-b4bc-6d23568f5aad","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":495973,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Zone of inhibition of the treated fabrics against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e. (b) Antibacterial properties of treated fabrics by plate counting method. (c) Killing efficiency of the treated fabrics against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus \u003c/em\u003e(d)\u003cem\u003e.\u003c/em\u003e\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/6533635d890eabdc142ebfe9.png"},{"id":65682181,"identity":"956689cd-0195-4ac4-8786-73d4d5e82748","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":167434,"visible":true,"origin":"","legend":"\u003cp\u003e(a) The inhibition zone of Cu@ZIF-L@Cotton fabric before and after being washed for 5 cycles,\u003cstrong\u003e \u003c/strong\u003e(b) WCAs of Cu@ZIF-L@Cotton fabric after 5 cycles washing.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/ac3462a9985410112766f7a4.png"},{"id":74858799,"identity":"9b911442-b712-49b9-82f6-9e3cf54b970c","added_by":"auto","created_at":"2025-01-27 16:12:59","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2976122,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/6a6af4f3-144d-4789-a356-21724f8e2926.pdf"},{"id":65682184,"identity":"19f255ec-d089-49af-b89a-a8112440f906","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"mp4","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":27517952,"visible":true,"origin":"","legend":"","description":"","filename":"MovieS1.mp4","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/94774c6cee58e4de5734b497.mp4"},{"id":65682183,"identity":"b2620a88-999a-41ff-92b7-64419377d443","added_by":"auto","created_at":"2024-10-01 09:01:01","extension":"docx","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":3694886,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/f2c023694786579bf7c6fc51.docx"},{"id":65682934,"identity":"e2636ea9-2840-4e6c-a3b5-77c31dddbff2","added_by":"auto","created_at":"2024-10-01 09:09:01","extension":"png","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":139684,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eScheme 1.\u003c/strong\u003e Fabrication scheme of MTMS/Cu@ZIF@Cotton fabrics.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-4975082/v1/9f8d018b051da2b2bd44e5c4.png"}],"financialInterests":"No competing interests reported.","formattedTitle":"ZIF-L coated cotton fabric for antibacterial and self-cleaning applications","fulltext":[{"header":"Introduction","content":"\u003cp\u003eBacterial infections pose an increasingly grave threat to public health, and effectively combating these threats on a large scale has become an uphill task (Halloran \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). Transmission via contaminated surfaces has been recognized as a significant pathway for spreading pathogenic microorganisms (Mallakpour et al. \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Nasri et al. \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). The COVID-19 pandemic has heightened global attention to the transmission of contamination facilitated by high-touch surfaces, for example, textiles, public transport, and so on (Imani et al. \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e2020a\u003c/span\u003e). In response, relevant researchers are currently investigating the utilization of surfaces and coatings that possess the capability to inhibit the proliferation and dissemination of microorganisms through either eradication or reduction of microbial adhesion to textile surfaces, given that textiles serve as high-contact materials. The achievement of these goals has been facilitated by the utilization of surface-bound active antimicrobials (Qiu et al. \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e2022\u003c/span\u003e), as well as the development of biocidal coatings (Ye et al. \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e2021\u003c/span\u003e) and passive pathogen-repellent surfaces employing nanomaterials (Imani et al. \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e2020b\u003c/span\u003e), chemical modifications, and micro- and nanostructuring techniques (Crawford et al. \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e2012\u003c/span\u003e; Shen et al. \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e2021\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eThe utilization of metal-organic frameworks (MOFs) nanostructures, exemplified by zeolitic imidazolate frameworks (ZIFs), holds immense potential due to their inherent antibacterial activity, in conjunction with their ability to function as a reservoir for metal ions (Zhuang et al. \u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e2012\u003c/span\u003e; Taheri et al. \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e2021\u003c/span\u003e). ZIF-L, formed by linking zinc ions and the organic ligand 2-methylimidazole (2-MI), exhibits the same structural unit as that of ZIF-8. Both ZIF-L and ZIF-8 possess good antibacterial properties, attributed to the release of Zn\u003csup\u003e2+\u003c/sup\u003e ions and imidazole-like antibacterial organic ligands (Yuan and Zhang \u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; He et al. \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e2023\u003c/span\u003e; Li et al. \u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). Furthermore, the nano-dagger arrays of ZIF-L prevent bacterial growth by rupturing the adhered microbial cells through their sharp tips (Yuan et al. \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). The ZIF-L nano-structure is typically grown \u003cem\u003ein situ\u003c/em\u003e on textile surfaces, and constructing the microstructures/nanostructures on the surface of substrates, thereby imparting antibacterial properties to the fabric and simultaneously enhancing its surface roughness. Despite these advances, there are still exit challenges that need to be addressed, particularly concerning the aggregation and poor durability of ZIF-L on textile surfaces.\u003c/p\u003e \u003cp\u003eMoreover, the recent emergence of self-cleaning cotton fabrics with antibacterial properties has garnered significant attention. Due to the abundant presence of hydroxyl groups on its surface, cellulose-based fibers exhibit high absorbency and are prone to staining when exposed to liquids(Xu et al. \u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e2010\u003c/span\u003e). Generally, there are two approaches to fabricating self-cleaning textiles. One approach involves the creation of a photocatalytic fabric with properties such as TiO\u003csub\u003e2\u003c/sub\u003e, which facilitates the decomposition of most stains on the fabric (Karimi and Esmail \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). The other approach focuses on preparing superhydrophobic fabrics that exhibit resistance towards various liquids, enabling easy removal of dirt from the fabric through water. The superhydrophobic surface can be achieved by combining the synergistic effects of low surface energy materials (fluoride, alkane) and rough hierarchical structures (micro-, nano-, or micro/nanostructures) (Wen et al. \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e2015\u003c/span\u003e; Li and Guo \u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Li et al. \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). Inspired by these results, we believe that taking advantage of the morphological evolution of ZIF-L to develop the hydrophobic structure is a promising strategy for constructing antibacterial and self-cleaning materials.\u003c/p\u003e \u003cp\u003eIn this study, we described a convenient approach for fabricating copper ion doping ZIF-L (Cu@ZIF-L) on cotton fabrics via an \u003cem\u003ein-situ\u003c/em\u003e growth method. By adjusting the molar ratio of 2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e and reaction time, both the quantity and morphology of ZIF-L could be modulated. Then, treatment with MTMS led to the formation of hydrophobic cotton fabric (MTMS/Cu@ZIF-L@Cotton). The antibacterial activities against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e were evaluated, along with investigations into hydrophobicity and self-cleaning properties. Additionally, functional stability after washing was also assessed.\u003c/p\u003e"},{"header":"Experimental","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003eMaterials\u003c/h2\u003e \u003cp\u003ePlain-woven cotton fabrics (120 g/m\u003csup\u003e2\u003c/sup\u003e) were purchased from Qinzhe Textiles Co., Ltd. 2-methylimidazole (2-MI), zinc chloride (ZnCl\u003csub\u003e2\u003c/sub\u003e) and Methyltrimethoxysilane (MTMS) were supported from Shanghai Macklin Biochemical Technology Co., Ltd. Copper chloride dihydrate (CuCl\u003csub\u003e2\u003c/sub\u003e) were purchased from Sinopharm Chemical Reagent Co., Ltd. All chemical reagents were used as received unless specified otherwise.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003eFabrication of ZIF-L@Cotton\u003c/h2\u003e \u003cp\u003eThe raw cotton fabrics were rinsed in ethanol and deionized (DI) water by sonication for 30 min as pretreated first. After drying, cotton fabrics were cut into 2 cm \u0026times; 5 cm and put into a ziplock bag for later use. The pretreated cotton fabric was immersed vertically in 200 mL of aqueous solution of 2-MI (0.35 M) for 30 min. After that, 20 mL of ZnCl\u003csub\u003e2\u003c/sub\u003e aqueous solution (0.5 M) was introduced dropwise. After stirring for 3 h, the cotton fabric was taken out, washed with ethanol and DI water, and then dried under vacuum at 65 ℃ to obtain ZIF@Cotton. In addition, other ZIF@Cotton with different molar ratios (2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e = 5:1) and different times (1h, 3h, and 5h) were prepared. The ZIF@Cotton (from 2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e = 7:1, 3 h) was used for further characterization.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003eFabrication of Cu@ZIF-L@Cotton\u003c/h2\u003e \u003cp\u003eCu@ZIF-L@Cotton was prepared as follows: the cotton fabric was placed vertically in the aqueous solution of 2-MI (0.35 M), and then the mixture of ZnCl\u003csub\u003e2\u003c/sub\u003e and CuCl\u003csub\u003e2\u003c/sub\u003e aqueous solution (4 M:1 M) was introduced dropwise to the above solution and kept still for another 3 h. Afterward, the fabric was removed, washed several times with ethanol and DI water, and then dried at 65 ℃ in an oven. Also, other Cu@ZIF@Cotton with different molar ratios (2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e = 5:1) and different times (1h, 3h, and 5h) were prepared. The Cu@ZIF@Cotton (from 2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e = 7:1, 3 h) was used for the following modification.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003eFabrication of MTMS/Cu@ZIF-L@Cotton\u003c/h2\u003e \u003cp\u003eThe hydrophobic method was followed according to a previous report (Fei et al. \u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e2022\u003c/span\u003e). The Cu@ZIF-L@Cotton sample and a petri dish containing MTMS were placed in a drying vessel. The drying vessel was sealed and then heated at 70 ℃ for 3 h. After that, unreacted MTMS was removed by placing the modified samples in a vacuum oven at 60 ℃ for 1 h. Hydrophobic cotton fabric (MTMS/Cu@ZIF-L@Cotton) was then achieved.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003eCharacterizations\u003c/h2\u003e \u003cp\u003eThe surface morphology and elemental compositions were examined using field emission scanning electron microscope (FE-SEM, Ultra-55, Carl Zesis, Germany) and energy dispersive spectrometer (EDS), respectively. The Fourier transform infrared spectroscopy (FT-IR, Nicolet 5700, Thermo Fisher Scientific, USA) data were collected in the range of 400\u0026mdash;4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. The composition was measured with the X-ray photoelectron spectrometer (XPS, K-ALPHA, Thermo Fisher Scientific, USA). The water contact angle (WCA) of the samples was measured using a Contact Angle Analyzer (JY-PHb, Bingjing, China) at room temperature.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eBacterial adhesion test\u003c/h2\u003e \u003cp\u003eThe cotton fabrics, before and after modification, were immersed in 25 mL of bacterial suspension (\u003cem\u003eS. aureus\u003c/em\u003e) containing 10\u003csup\u003e7\u003c/sup\u003e CFU mL\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and incubated under static conditions at 37 ℃ for 2 h. Subsequently, the fabrics were taken out and held vertically for 3 min to allow any remaining droplets to slide away. Following this, the fabrics were washed twice with 5 mL of sterile water to remove any unadhered bacteria. Next, the cotton fabrics were fixed with 2.5% glutaraldehyde solution for 2 h at 4 ℃ and then rinsed twice with PBS. Afterward, the samples were dehydrated using a series of graded ethanol solutions (50, 75, 90, and 100 wt %, for 15 min each) and then observed under SEM after drying and treatment with platinum.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003eAntibacterial test\u003c/h2\u003e \u003cp\u003eGram-negative \u003cem\u003eEscherichia coli\u003c/em\u003e (\u003cem\u003eE. coli\u003c/em\u003e) and Gram-positive \u003cem\u003eStaphylococcus aureus\u003c/em\u003e (\u003cem\u003eS. aureus\u003c/em\u003e) were chosen for the antibacterial activity assessment by the zone of inhibition (ZOI) and shaking flask plate method. The cotton fabrics were cut into circular samples with a radius of 1 cm. A 200 \u0026micro;L of bacterial suspension (10\u003csup\u003e5\u003c/sup\u003e CFU/mL) was plated onto the LB agar plates. The cotton fabrics were placed on the surface of the LB agar and incubated at 37 ℃ for 24 h. The pristine cotton fabric was used as control.\u003c/p\u003e \u003cp\u003eThe shaking flask plate method was performed as follows, bacteria were diluted to approximately\u0026thinsp;~\u0026thinsp;10\u003csup\u003e5\u003c/sup\u003e CFU mL\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e in PBS (70 mL). The cotton fabric samples (0.75\u0026thinsp;\u0026plusmn;\u0026thinsp;0.05 g) were cut into pieces and added to the bacterial suspension, which was incubated at 37 ℃ for 24 h with shaking at 130 rpm. After that, 100 \u0026micro;L of culture medium was removed and serially diluted to the appropriate dilution before plating onto LB agar plates. The bacteria were incubated at 37 ℃ for 24 h. After that, the number of bacterial colonies on the plates was counted and the killing rate was evaluated using the following equation:\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e\n$$\\:Antibacterial\\:Rate=({C}_{control}-{T}_{sample})/{C}_{control}\\times\\:100$$\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003ewhere \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:{C}_{control}\\)\u003c/span\u003e\u003c/span\u003e is the number of bacterial colonies of the control sample; \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:{T}_{sample}\\)\u003c/span\u003e\u003c/span\u003e is the number of bacterial colonies of the treated cotton fabrics.\u003c/p\u003e \u003c/div\u003e"},{"header":"Results and discussion","content":"\u003cp\u003eIn this study, a hydrophobic antibacterial cotton fabric was achieved via a simple \u003cem\u003ein-situ\u003c/em\u003e deposition method, as shown in Scheme \u003cspan refid=\"Sch1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. First, the cotton fabric was vertically immersed in a precursor solution containing 2-MI. Upon the addition of ZnCl\u003csub\u003e2\u003c/sub\u003e or ZnCl\u003csub\u003e2\u003c/sub\u003e/CuCl\u003csub\u003e2\u003c/sub\u003e, simultaneous nucleation and crystal growth took place on the cotton fabrics. Alternatively, Cu\u003csup\u003e2+\u003c/sup\u003e could form coordination with dimethylimidazole; however, its binding affinity was comparatively weaker than that of Zn\u003csup\u003e2+\u003c/sup\u003e (Yang et al. \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). During this process, ZIF-L or Cu@ZIF-L formed and deposited on the fabric surface, which could be attributed to electrostatic and coordination interaction between the hydroxyl groups of cellulose and Zn\u003csup\u003e2+\u003c/sup\u003e/Cu\u003csup\u003e2+\u003c/sup\u003e ions (Yang et al. \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). The Cu@ZIF-L@Cotton fabric was subsequently subjected to chemical vapor deposition of MTMS for surface modification, aiming to achieve a low-energy state and thereby obtain a hydrophobic cotton fabric.\u003c/p\u003e \u003cp\u003eThe surface morphology structure of the pristine and modified cotton fabrics was characterized by SEM. As shown in Figure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e, the pristine cotton fabric has a smooth surface. When ZIF-L or Cu@ZIF-L were formed and \u003cem\u003ein-suit\u003c/em\u003e grew on the surface of cotton fabric, the surface morphology of cotton fibers was changed obviously. As shown in Figs.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea and b, the coated cotton fabric was covered by a thick layer of ZIF-L or Cu@ZIF-L nano-dagger. Each nano-dagger resembled a vertically extending sharp-tipped leaf, intricately arranged on the cotton fabric surface and fully covered the substrates. These structures correspond to the characteristic appearance of the ZIF-L nanostructure. The observed vertical alignment could primarily be attributed to the confined growth of ZIF-L, wherein the complete coverage of cotton fiber by small ZIF-L crystals leads to the subsequent appearance of larger ZIF-L crystals during continuous growth. As indicated by the red arrows, the ZIF scattered on the fabric surface reveals nano-dagger with dimensions of ~\u0026thinsp;2 \u0026micro;m in width and ~\u0026thinsp;6 \u0026micro;m in height. By adjusting the molar ratio of 2-MI/Zn\u003csup\u003e2+\u003c/sup\u003e and reaction time, the amount and morphology of the ZIF-L could be changed (Figure \u003cspan refid=\"MOESM2\" class=\"InternalRef\"\u003eS2\u003c/span\u003e). When the amount of 2-MI was low, the surface coverage of the fabric appeared incomplete or the structure of the surface layer was indistinct. With an increase in the content of 2-MI and reaction time, both the size and density of ZIF-L or Cu@ZIF-L exhibit a corresponding increase. Notably, as shown in Figure S3, for Cu@ZIF-L, at a molar ratio of 2-MI to Zn\u003csup\u003e2+\u003c/sup\u003e equal to 5, a relatively sparse distribution of Cu@ZIF-L was observed on the fabric surface. When the ratio of 2-MI to Zn\u003csup\u003e2+\u003c/sup\u003e reached 7:1, the dense and uniform layer of Cu@ZIF-L be achieved. After MTMS modification, it could be observed that the morphological structure is unchanged compared with Cu@ZIF-L@Cotton fabric, and it was still coated with a tight nano-dagger structure (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec). The chemical composition of samples was characterized using EDS mapping. In the case of ZIF@Cotton, C, O, N, and Zn elements were detected (Figure S4a). Additionally, Cu element was observed in Cu@ZIF@Cotton along with the aforementioned elements found in ZIF@Cotton (Figure S4b). These results further confirmed the successful formation of ZIF-L or Cu@ZIF-L on the surface of cotton fibers. Furthermore, EDS analysis revealed that MTMS/Cu@ZIF-L@Cotton exhibited surface elements including C, O, N, Zn, Cu, and Si (from MTMS) (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed). Notably, these elements were uniformly distributed on the surface of fabric fibers, so it could be proved that MTMS was well attached to the surface of the Cu@ZIF-L@Cotton.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe chemical composition of different samples was characterized by FT-IR, which was depicted in Figs.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea and b. For ZIF-L and Cu@ZIF-L, the absorption peak at 3100 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 2920 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e belonged to the aromatic and aliphatic C-H stretch of imidazole, respectively. The peak observed at 1147 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e corresponded to the C-N stretching vibration of imidazole linkers in ZIF-L. The strong absorption bands detected at 757 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 690 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e could be attributed to the out-of-plane bending of the Hmim ring, while the band observed at 1308 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e was associated with the in-plane bending (Zhang et al. \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). The band observed at 1567 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e corresponded to the C\u0026thinsp;=\u0026thinsp;N double band stretching vibration. Furthermore, the absorption peak around 420 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e signified the Zn-N stretching mode of the formed ZIF-L, indicating the coordination of Zn\u003csup\u003e2+\u003c/sup\u003e with nitrogen atoms in 2-MI to form imidazolate(Bustamante et al. \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e2014\u003c/span\u003e). The absorption peak at about 550\u0026ndash;620 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e belonged to the Cu-N bond, which was observed on the spectrum of Cu@ZIF-L (Yang et al. \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). This suggested the successful embedding of Cu \u003csup\u003e2+\u003c/sup\u003e on ZIF-L. As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, the pristine cotton fabric exhibited only two main characteristic peaks at 2901 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 3320 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, corresponding to the stretching vibrations of C-H and -OH groups, respectively. After the deposition of ZIF-L and Cu@ZIF-L, distinct characteristic peaks attributed to ZIF-L and Cu@ZIF-L emerged, indicating the successful growth of these materials on the cotton substrate. After the silane modification, the MTMS/Cu@ZIF-L@Cotton exhibited two new characteristic peaks at 1262 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 801 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, attributed to Si-CH\u003csub\u003e3\u003c/sub\u003e and Si-O-Si, indicating the formation of a siloxane network (Qin et al. \u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e2021\u003c/span\u003e; Fan et al. \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e2023\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eTo further determine the chemical composition changes of fabrics at each modification step, the XPS testing was performed to further study the elemental composition and valence of the related samples. In the wide-scan XPS spectrum of pristine cotton fabric, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec, only peaks corresponding to C1s and O1s were observed. Upon deposition of ZIF-L, three additional peaks emerged at 1044.58 eV, 1021.62 eV, and 400.09 eV, which could be attributed to Zn 2p 1/2, Zn 2p 3/2, and N1s states respectively (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed) (Ananth et al. \u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e2017\u003c/span\u003e; Wang et al. \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). After depositing Cu@ZIF-L, resulted in the appearance of Cu 2p peaks in addition to the aforementioned ones. The high-resolution spectrum of Cu 2p was divided into three parts (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee), in which the peaks centered at approximately 953.18 and 933.35 eV correspond to Cu 2p 1/2 and Cu 2p 3/2, respectively (Li et al. \u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e2019\u003c/span\u003e). Additionally, it is noteworthy that two satellite peaks were observed at 944.48 and 940.82 eV, indicating the predominant presence of the Cu\u003csup\u003e2+\u003c/sup\u003e valence state (Elfeky et al. \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e2019\u003c/span\u003e; Sun et al. \u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e2020\u003c/span\u003e). In addition, the deconvolution of N 1s revealed three distinct peaks at 407.50, 400.08, and 398.75 eV (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef), corresponding to the N\u0026thinsp;=\u0026thinsp;C, N\u0026thinsp;\u0026minus;\u0026thinsp;Zn \u0026amp; N\u0026thinsp;\u0026minus;\u0026thinsp;Cu, and N\u0026thinsp;\u0026minus;\u0026thinsp;C bonds respectively (Bhattacharyya et al. \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2016\u003c/span\u003e; Yang et al. \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e2023\u003c/span\u003e). Furthermore, after coating with MTMS, two new peaks around 101.0 (Si 2p) and 154.4 (Si 2s), indicating that Cu@ZIF-L@Cotton fabric was covered by MTMS (Yang et al. \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e2021\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe wettability of a material's surface is comprehensively determined by its chemical composition, surface roughness, and surface energy(Campoccia et al. \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e2013\u003c/span\u003e). Measurement of the water contact angle (WCA) is widely employed to characterize the surface wettability of materials. The WCA of the original cotton fabric was 0\u0026deg;, indicating a good hydrophilic (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). After surface modification by in-situ grown ZIF-L or Cu@ZIF-L, the WCA of the ZIF-L@Cotton and Cu@ZIF-L@Cotton fabric was still 0\u0026deg; on the basis of the increased surface roughness (Figs.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb and c). The subsequent modification of MTMS on the Cu@ZIF-L@Cotton enhanced the hydrophobicity with a WCA of 132\u0026deg;\u0026thinsp;\u0026plusmn;\u0026thinsp;0.58 (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed). The synergy between nanostructures and low surface energy contributes to the good hydrophobic performance of this material. In addition, water droplets repel the fabric surface when the contact angle is tested, which also illustrates the hydrophobicity of the sample surface (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee and Movie S1). Furthermore, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef, four kinds of droplets including dyed red water, milk, coffee, and juice steadily stood on the surface of Cu@ZIF-L@Cotton fabric displaying good anticontamination and water-resistant properties. To investigate the self-cleaning capability of the as-prepared fabric, the surface of Cu@ZIF-L@Cotton was contaminated with Congo red dye powders. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg, water droplets could roll easily away from the surface carrying away the Congo red dye from the fabric surface. Therefore, the as-prepared Cu@ZIF-L@Cotton fabric showed good self-cleaning performance.\u003c/p\u003e \u003cp\u003eFurthermore, Gram-positive \u003cem\u003eS. aureus\u003c/em\u003e was selected as the representative microorganism to explore the bacterial repellency properties. The adherence of bacteria on cotton, Cu@ZIF-L@Cotton, and MTMS/Cu@ZIF-L@Cotton fabrics was observed by SEM as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eh. For cotton fabric, large amounts of bacteria adhere to the raw cotton fabric surface. Cu@ZIF-L@Cotton fabric also exhibited a significant adherence of \u003cem\u003eS. aureus\u003c/em\u003e to the Cu@ZIF-L nanostructures. On one hand, the positive electrical property of Cu@ZIF-L enabled it to attract negatively charged bacteria. On the other hand, owing to its metal ion core and unsaturated nitrogen from the organic linker, Cu@ZIF-L exhibited an affinity for amino acid residues (Tanum et al. \u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e2022\u003c/span\u003e), which are abundant in peptidoglycan-the main component of \u003cem\u003eS. aureus\u003c/em\u003e cell wall (Romaniuk and Cegelski \u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e2015\u003c/span\u003e) (Nikolic and Mudgil \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e2023\u003c/span\u003e)-thus facilitating its attraction towards bacteria. While in the MTMS/Cu@ZIF-L@Cotton fabric, the adhered bacteria were reduced. The hydrophobicity surface demonstrated the repelling effect against bacteria, those tenacious bacteria that managed to be in touch with the surface were killed by Cu@ZIF-L itself.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe antibacterial performance of as-prepared Cu@ZIF-L@Cotton fabric was evaluated using the agar diffusion plate method and shake flask method against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e. As displayed in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea and Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, without inhibition zone around the pristine cotton was observed for \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e. For ZIF-L@Cotton and Cu@ZIF-L@Cotton fabric, obvious inhibition zones were seen against all of the strains compared to the uncoated sample fabric. However, after MTMS coating, the distinct inhibition zone was still observed except for a slight decrease against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e, which might be attributed to the prohibition of the diffusion of Zn\u003csup\u003e2+\u003c/sup\u003e and Cu\u003csup\u003e2+\u003c/sup\u003e by hydrophobic treatment.\u003c/p\u003e \u003cp\u003eThe shaking flask method was also employed to assess their antibacterial activities. As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb, the ZIF-L@Cotton, and Cu@ZIF-L@Cotton fabrics exhibited pronounced antibacterial properties compared to the pristine cotton fabric. The antibacterial efficacy of the ZIF-L@Cotton fabric against \u003cem\u003eS. aureus\u003c/em\u003e was significantly superior to that against \u003cem\u003eE. coli\u003c/em\u003e, owing to the absence of an outer membrane in Gram-positive bacteria (\u003cem\u003eS. aureus\u003c/em\u003e), rendering them more susceptible to destruction as opposed to Gram-negative bacteria (\u003cem\u003eE. coli\u003c/em\u003e) with their dual-membrane structure separated by peptidoglycan (Han et al. \u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e2018\u003c/span\u003e). Remarkably, the Cu@ZIF-L@Cotton fabric demonstrated exceptional antibacterial activities, achieving a 5 log CFU reduction of both \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e, indicating a promising killing efficacy of 99.999%. Consequently, doping Cu\u003csup\u003e2+\u003c/sup\u003e into ZIF-L enhanced the antibacterial properties of the fabric considerably. Furthermore, it was worth noting that the antibacterial properties of the sample remained unaffected by modification through MTMS, as evidenced by the absence of bacterial growth on the agar plate. The MTMS/Cu@ZIF-L@Cotton fabric exhibited remarkable antibacterial properties and self-cleaning capabilities, effectively killing tenaciously adhered bacteria on its surface due to the exceptional antibacterial efficacy of Cu@ZIF-L.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eZone of inhibition (mm) of samples.\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"5\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eMicroorganism\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePristine Cotton\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eZIF-L@Cotton\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eCu@ZIF-L@Cotton\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eMTMS/Cu@ZIF-L@Cotton\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cem\u003eE. coli\u003c/em\u003e/mm\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e0\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e10.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e10.3\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e5.8\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cem\u003eS. aureus\u003c/em\u003e/mm\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e \u003cp\u003e0\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e11.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e \u003cp\u003e12.9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e8.8\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eThe functional stability of the as-prepared cotton fabric against washing was evaluated by testing the changes in the inhibition zone and WCA. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea, the Cu@ZIF-L@Cotton fabric still displayed an obvious inhibition zone after undergoing washing, indicating its good antibacterial activity. In addition, the WCA of the Cu@ZIF-L@Cotton fabric was still above 120\u0026deg; after undergoing five laundering cycles. These results indicated that the cotton fabric prepared in this study exhibited good functional stability.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e"},{"header":"Conclusion","content":"\u003cp\u003eIn summary, antibacterial and self-cleaning properties were imparted to cotton fabrics by \u003cem\u003ein-situ\u003c/em\u003e growth of Cu@ZIF-L nanostructures on their surface, followed by modification using MTMS via chemical vapor deposition (MTMS/Cu@ZIF-L@Cotton). Dagger-like ZIF-L nanostructures were vertically grown on the cotton surface, effectively addressing agglomeration issues. The incorporation of Cu\u003csup\u003e2+\u003c/sup\u003e ions enhanced the antibacterial efficacy, demonstrating remarkable antimicrobial activity against \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus\u003c/em\u003e by achieving 5-log of CFU reduction for both bacterial strains. Moreover, the prepared cotton fabric exhibited hydrophobicity and excellent self-cleaning properties. Additionally, these fabricated fabrics demonstrated good functional stability even after 5 washing cycles. The obtained positive outcomes indicate that the developed cotton fabric exhibits great potential as a promising candidate for various applications in the biomedical field.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eFunding\u0026nbsp;\u003c/strong\u003eWe acknowledge financial support from the Zhejiang Provincial Natural Science Foundation of China (Grant No. LQ23E030012); and the Scientific Research Foundation of Zhejiang Sci-Tech University (Grant No. 22202001-Y).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contributions\u0026nbsp;\u003c/strong\u003eQiaohua Qiu: Conceptualization; Methodology; Data curation; Writing. LiYing Lan: Material preparation; Data collection.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u0026nbsp;\u003c/strong\u003eData can be available from the corresponding author ([email protected]) upon academic reasonable request.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eConflict of interest\u003c/strong\u003e The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eEthical approval and consent to participate\u003c/strong\u003e This article does not contain any studies with human participants or animals performed by any of the authors.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n \u003cli\u003eAnanth A, Dharaneedharan S, Seo HJ, et al (2017) Soft jet plasma-assisted synthesis of Zinc oxide nanomaterials: Morphology controls and antibacterial activity of ZnO. 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Adv Healthc Mater 1:225\u0026ndash;238. https://doi.org/10.1002/adhm.201100043\u003c/li\u003e\n\u003c/ol\u003e"},{"header":"Scheme","content":"\u003cp\u003eScheme 1 is available in the Supplementary Files section.\u003c/p\u003e\n"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"cellulose","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"cels","sideBox":"Learn more about [Cellulose](https://www.springer.com/journal/10570)","snPcode":"10570","submissionUrl":"https://submission.nature.com/new-submission/10570/3","title":"Cellulose","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"ZIF-L, cotton, MTMS, antibacterial, self-cleaning","lastPublishedDoi":"10.21203/rs.3.rs-4975082/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4975082/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eTextiles that possess antibacterial and self-cleaning properties play a crucial role in preventing the growth and spread of microbes. Zeolitic imidazolate framework-L (ZIF-L) nanostructures have gained significant attention in research due to their ability to sustainably release Zn\u003csup\u003e2+\u003c/sup\u003e ions, coupled with the physical destruction of bacteria by their blade tips. Integrating natural fabrics with ZIF-L represents an effective approach to enhancing the value-added features of textiles with unique functionalities. In this study, we reported a facile technology for the \u003cem\u003ein-situ\u003c/em\u003e growth of ZIF-L on cotton fabrics. A uniform and dense coating of leaf-shaped nanostructures by doping Cu\u003csup\u003e2+\u003c/sup\u003e ions on ZIF-L was formed on the cotton fiber surface (Cu@ZIF-L@Cotton), followed by treatment with methyltrimethoxysilane (MTMS) to obtain water-repellent MTMS/Cu@ZIF-L@Cotton fabric. The resulting fabrics exhibited excellent antibacterial activities against both Gram-negative and Gram-positive bacteria, effectively killing 5 log CFU (\u0026gt;99.999%) of \u003cem\u003eE. coli\u003c/em\u003e and \u003cem\u003eS. aureus.\u003c/em\u003e Furthermore, the prepared cotton fabric not only showed hydrophobicity with a water contact angle of 132\u0026deg;\u0026thinsp;\u0026plusmn;\u0026thinsp;0.58 but also displayed good self-cleaning properties. Additionally, these fabricated fabrics showed good functional stability after washing. It is therefore believed these valuable functions could significantly enhance the practical feasibility of the fabric in various application scenarios.\u003c/p\u003e","manuscriptTitle":"ZIF-L coated cotton fabric for antibacterial and self-cleaning applications","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-10-01 09:00:56","doi":"10.21203/rs.3.rs-4975082/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-09-01T19:33:40+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-08-31T13:13:50+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-08-31T13:13:14+00:00","index":"","fulltext":""},{"type":"submitted","content":"Cellulose","date":"2024-08-26T04:00:50+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"cellulose","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"cels","sideBox":"Learn more about [Cellulose](https://www.springer.com/journal/10570)","snPcode":"10570","submissionUrl":"https://submission.nature.com/new-submission/10570/3","title":"Cellulose","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"ca60d14e-1b9e-47a8-9afd-7c4022dd4046","owner":[],"postedDate":"October 1st, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2025-01-27T16:07:49+00:00","versionOfRecord":{"articleIdentity":"rs-4975082","link":"https://doi.org/10.1007/s10570-025-06400-6","journal":{"identity":"cellulose","isVorOnly":false,"title":"Cellulose"},"publishedOn":"2025-01-24 15:57:06","publishedOnDateReadable":"January 24th, 2025"},"versionCreatedAt":"2024-10-01 09:00:56","video":"","vorDoi":"10.1007/s10570-025-06400-6","vorDoiUrl":"https://doi.org/10.1007/s10570-025-06400-6","workflowStages":[]},"version":"v1","identity":"rs-4975082","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4975082","identity":"rs-4975082","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}