Introduction

Mangifera indica (mango), a tropical fruit belonging to the genus Mangifera in the family Anacardiaceae, is widely cultivated in tropical regions around the world1. The species, known as M. indica, holds significant value in Ayurvedic medicine, where its various parts are attributed with different medicinal properties2. Studies have demonstrated that M. indica root extracts possess antibacterial3 and anti-inflammatory4 properties, while its bark exhibits diuretic effects5. Mango peels, a major by-product of mango processing industries, account for 15–20% of the total fruit weight. The primary polyphenolic constituents of mango peel include mangiferin, quercetin, rhamnetin, ellagic acid, kaempferol, and their related conjugates6. Research indicates that mango peels exhibit antioxidant, antibacterial, and antifungal properties7,8,9.

Plant-based nanoparticle synthesis, which employs plant extracts as reducing and capping agents, has gained significant attention in recent decades due to its environmental sustainability, simplicity, and high yield production10,11 as compared to chemical and other biological method of nanoparticle synthesis like that of the use of bacteria or fungi. Gold nanoparticles (AuNPs), known for their biocompatibility12,13, are synthesized from various plant parts14,15,16,17,18,19,20,21. Researchers have successfully produced AuNPs using aqueous leaf extracts from Populus alba14 and Phragmites australis15, as well as peel extracts from Garcinia mangostana16 and Citrus maxima17,18. Extracts from Amorphophallus paeoniifolius19, tarragon20, Clitoria ternatea21, Croton sparsiflorus22, and bark of Mimusops elengi23 have also been used for AuNP synthesis. Plant-synthesized AuNPs have demonstrated various applications, including antibacterial23, antifungal24, antioxidant25, catalytic26, and anticancer properties27.

The dyeing of textiles presents significant environmental challenges, particularly with the use of synthetic dyes containing harmful chemicals28. The dyeing process contributes to pollution of air, water, and soil, with untreated effluents harming ecosystems and potentially causing mutagenic cancers in organisms exposed to contaminated environments29.

Noble metal nanoparticles, such as silver and gold, have shown great potential as colorants, offering a promising alternative for coloring organic materials30. Their surface plasmon resonance properties enable them to impart vibrant and stable colors to fabrics. For instance, Johnston et al. developed a novel method for coloring wool using nanogold, resulting in a deep purple hue even with minimal gold nanoparticle deposition31. Similarly, Wu and colleagues synthesized silver nanoparticles with finely tuned surface plasmon resonance characteristics, successfully producing red, blue, yellow, orange, and violet hues on cotton fabrics32. Hasan et al. achieved brilliant coloration of nylon fabrics in red, yellow, and blue by varying reagent concentrations during silver nanoparticle synthesis, creating durable colors suitable for wearable conditions33.

In addition to providing vibrant and stable coloration, nanoparticle integration into fabrics also imparts functional properties, such as antibacterial activity. Tang et al. demonstrated that in-situ synthesized gold nanoparticles on silk exhibited antibacterial properties against E. coli34. Similarly, gold nanoparticles synthesized using Citrus limon extract and applied to cotton fabric showed antibacterial effects against S. aureus and E. coli bacterial strains35. Silver nanoparticles synthesized with chitosan imparted antibacterial properties to organic cotton fabric, effectively reducing E. coli and S. aureus bacterial growth36. Abolassad et al. impregnated cotton with silver and zinc oxide nanoparticles, achieving a > 95% reduction in bacterial colonies37. Elmaaty et al. reported significant antibacterial activity of selenium nanoparticles on wool against both gram-positive and gram-negative bacteria38.

To date, the integration of nanomaterials into fabrics for antimicrobial properties remains an emerging technology for specific applications. The use of AuNPs synthesized from M. indica fruit peel as both a colorant and an antibacterial agent for cotton has not been reported elsewhere. In this study, plant-synthesized AuNPs derived from M. indica fruit peel extract, were used to dye cotton fabric and investigate its antibacterial properties. The AuNP-dyed cotton threads were tested for color fastness and resistance to fading under various harsh conditions. This work highlights the potential of AuNP-dyed cotton threads for applications in the fabric-based biomedical industry.

Materials and methods

Reagents

Gold (III) chloride hydrate (HAuCl4) (99.995% trace metals basis) was purchased form Merck and was diluted with ultrapure water to produce 10 mM HAuCl4. Ultrapure water (18.2 mΩ, Direct-Q, Millipore SAS) was used for the dilution of HAuCl4. Methanol (100% anhydrous assay VWR) was used for the extraction of mango peels.

Apparatus

Erlenmeyer flask (100 mL) was used for the synthesis of gold nanoparticle as well as micropipettes, watch glass, weights, magnetic stirrer, mercury thermometer, and hot plate were used for gold nanoparticle synthesis via mango peel extract.

Preparation of fruit peel extract. Mango fruits were purchased from a local market in Iligan City, Philippines. The peels were collected and dried at room temperature until constant weight and then methanol was added. Methanol was used for the extraction process due to its polar nature, which ensures superior performance in extracting biomolecules from plants39. After a week, the mixture was filtered to produce the mango peel extract solution.

Green synthesis of gold nanoparticles. The AuNP solutions were synthesized by reducing HAuCl₄ (gold ion) with M. indica fruit peel extract. Different colors of AuNP solutions were obtained by varying the initial concentrations of the gold ion solution. To achieve the desired concentrations, a 10 mM gold ion stock solution was diluted with ultrapure water to produce concentrations of 0.01, 0.1, 0.25, 0.50, 0.75, and 1 mM. Each gold ion solution had a total volume of 50 mL. For the synthesis process, gold ion solutions were poured into 100 mL Erlenmeyer flask, heated on a hotplate at 120 °C for 10 min, and stirred continuously at 360 rpm. After 10 min, the temperature of the gold ion solution was measured by a mercury thermometer at 55 °C. The reduction reaction began with the addition of 1 mL of mango peel extract, and the process continued for 10 min. The formation of AuNP was visually indicated by a color change from light yellow to shades of pink or dark violet, depending on the gold ion concentration.

Characterization of gold nanoparticles. The characteristic absorption peaks of the synthesized AuNPs were monitored by a Perkin Elmer Lambda 35 UV–Vis Spectrophotometer with a wavelength range of 200 nm to 1100 nm. The hydrodynamic sizes of the synthesized AuNPs were assessed using a Microtrac MN420 Nanotrac Wave II DLS equipment. FTIR was employed to determine functional groups present in the gold nanoparticles. The colloidal AuNP solution was centrifuged at 16,000 rpm for 1 h and 30 min prior to the FTIR test in the wave region of 400–4000 cm−1. Transition Electron Microscopy was performed to examine the shape and size of the nanoparticle synthesized using the green synthesis technique.

Dyeing of cotton with gold nanoparticles. The AuNP solutions were introduced into the fabric by thermo fixing method. First, the synthesized AuNP solutions were heated in a beaker to 85°C.  Subsequently, 20 pieces of cotton thread, of 1 inch in length each, were simultaneously added into the solution and heated with the AuNP solution. The threads were washed three times with ultrapure water and were dried at room temperature afterwards.

Characterization of AuNP dyed cotton. The AuNP dyed cotton samples underwent scanning electron microscopy using a JEOL JSM–6510LA analytical scanning electron microscope and FTIR spectrometry.

Color fastness of the fabrics. Different sets of AuNP dyed cotton samples were submerged in 1% acetic acid, 1% NaOH and detergent solution with pH 10.5 for 20 min each test. Color fastness was assessed by comparison between the tested fabric and the untested fabrics.

Antimicrobial disk diffusion assay. Pristine cotton and AuNP dyed cotton threads were evaluated against two pathogenic microorganisms (Escherichia coli and Staphylococcus aureus). The preparation of bacterial culture and inoculum, as well as the disk diffusion test, were conducted using the Mueller-Hilton agar (MHA), following the protocol stipulated in the CLSI document M02-A12 (CLSI, 2015). Three AuNP dyed cotton threads were then added to the plate. For positive controls, streptomycin was used for bacteria. Pristine cotton served as negative control. The plates inoculated with bacteria were incubated at 37 °C for 24 and 48 h, respectively. The zones of inhibition (ZOI) were carefully measured.

Results and discussion

Green synthesis and characterization of gold nanoparticles

Visual observation. The identification of gold nanoparticle (AuNP) formation relies on monitoring color changes in the solution during synthesis. In the experiment the gold ion solution turned red upon the addition of mango peel extract, indicating formation of AuNPs shown in Fig. 1a and b. The synthesized AuNP with different concentration appeared as having varying shades of red due to localized surface plasmon resonance40. This observation underscores the influence of gold ion concentration on the color of AuNPs which was used to imbue different shades of the color red into the cotton fabrics.

Fig. 1
figure 1

Gold solution (a), gold nanoparticle (b) colloidal solution and (c) UV–Vis spectra of the synthesized AuNPs by M.indica peel extract at various concentrations.

UV–vis spectrophotometer analysis. The UV–visible spectroscopy plays a crucial role in assessing gold nanoparticle (AuNP) synthesis across different gold ion concentrations. The prominent peaks in the visible spectrum marked the successful synthesis of AuNPs using the prepared M.indica fruit peel extract. The AuNPs ranging from 0.1 to 1.0 mM exhibit distinctive peaks aligning with typical gold nanoparticle localized surface plasmon peaks shown in Fig. 1c. The sharp peak at 530 nm is the characteristic peak of monodispersed spherical gold nanoparticles41. These results highlight excellent power of the prepared M.indica peel extract for stynthesizing AuNPs from various gold ion concentration.

Hydrodynamic diameter measurement. Dynamic light scattering (DLS) measurements revealed that the synthesized AuNPs developed hydrodynamic diameter within the nanometer scale as presented in Fig. 2. The different concentrations exhibited varying hydrodynamic dimensions, with 0.1 mM, 0.25 mM, and 0.50 mM concentrations showing sizes of 72, 60 and 51 nm respectively. Interestingly, concentrations of 0.75 mM and 1 mM resulted in smaller hydrodynamic diameters, both having 43 nm. These results highlight the successful synthesis of AuNPs having hydrodynamic diameters within the nanometer scale, with the use of M.indica fruit peel extract.

Fig. 2
figure 2

Hydrodynamic diameter of the synthesized AuNPs with different concentrations.

Transmission Electron Microscopy Images. Notably, the TEM image and the EDS graph in Fig. 3 confirms the successful synthesis of gold nanoparticles facilitated by the mango peel extract. The shape distribution is comprised mainly of spherical nanoparticles, with very few to no appearance of other shapes, like rods or triangles. The mean size of the nanoparticle with initial concentration of 0.25 mM gold ion solution is 16.90 nm. Further, Fig. 3b showed peaks for Au in the spectra which further confirms the synthesis of AuNP by using mango peel extract.

Fig. 3
figure 3

(a) TEM image of 0.25 AuNP and (b) corresponding EDS graph.

Fourier transform infra-red spectroscopy. The FTIR spectrum of 0.25AuNP is presented in Fig. 4. Pre-concentration of the solution through a centrifugation process was applied before testing. The functional groups responsible for the synthesis of AuNP are denoted by the corresponding peaks arising due to the infrared radiations. The functional groups that correspond to the peaks in the FTIR spectra of the AuNP are presented in Table 1.

Fig. 4
figure 4

FTIR spectra of 0.25AuNP.

Table 1 Prominent functional groups present in 0.25AuNP.

Nuclear magnetic resonance spectroscopy of the mango peel extract. Nuclear magnetic resonance peaks for the mango peel extract is presented in Fig. 5a and b. Flavonoids and their glycoside derivatives are found to be present in the M. indica peel extract including the catechins, quercetin, mangiferin, kaempferol, and rhamnetin42. These compounds are responsible for the antioxidant, antimicrobial, anti-inflammatory, antidiabetic, and anticarcinogenic activities of the peel extract. In this study, we were able to characterize the presence of flavonoids in the M. indica extract using NMR spectroscopy. The 1H NMR spectrum presented in Fig. 5a showed aromatic peaks at δ 6.20–7.40 which are attributed to the flavonoid aromatic protons. The 1H spectrum also showed signals in δ 3.20–5.40 which may be attributed to sugar moieties attached to the aglycone unit of a flavonoid glycoside. The flavone and sugar moieties were also corroborated in the 13C NMR spectra in Fig. 5b. Aromatic carbons were deduced at δ 90.0–165 while the probable sugar carbon signals were shown at δ 60.0–80.0.

Fig. 5
figure 5

(a) 1H-NMR of M. indica fruit peel extract (CD3OD, 600 MHz) and (b) 13C-NMR of M. indica peel extract (CD3OD, 150 MHz).

Reduction of AuNP via M. indica fruit peel extract

Figure 6 illustrates the potential reaction pathway between AuNP and the M. indica fruit peel extract. Flavonoids in the extract interact with AuNP by donating electrons through their phenolic groups and keto-enol tautomerism. In their enol form, the flavonoids break the O–H bond, releasing reactive hydrogen atoms that reduce Au3⁺ ions to Au0. This reduction facilitates the formation of AuNP. Following the reduction process, the resulting organic compounds likely act as nucleation units during the synthesis process depicted in Fig. 6.

Fig. 6
figure 6

(a) balanced chemical reaction of flavonoid and Chloroauric acid, (b) reduced gold ion capped with 2 flavonoid molecules.

Parameters like synthesis temperature, light, concentration of extract and pH affect the characteristics of AuNP. Here the UV–vis spectra of 0.25AuNP synthesized with varying synthesis temperature of 27 °C, 55 °C and 95 °C is presented in Fig. 7a. Different temperature during synthesis lead to a variation of UV–vis peaks, similar to what was observed by Tripathi et al.43. Lighting was varied during synthesis but it does not have any effect on the UV–vis spectra (Fig. 7b). Also, varying the amount of mango peel extract in the synthesis only affected the absorption intensity and no further increase in the intensity was observed as the volume increase from 1 to 2 ml (Fig. 7c). pH is also an essential factor and it has been reported that changes in pH result into the shift in the intensity44 as well as the shift in absorbance peak of the synthesized nanoparticle45. The work of Keijok et al. developed a controlled and reproducible method for synthesizing gold nanoparticles using Coffea arabica extract, optimizing synthesis temperature and pH through factorial design. They were able to successfully synthesized nearly uniform-sized AuNPs46.

Fig. 7
figure 7

UV–vis spectra of 0.25AuNP (a) with varying synthesis temperatures (b) with varying lighting condition and (c) with varying amount of mango peel extract (50:0.5 for instance is AuNP to extract volume ratio).

The reproducibility and stability of AuNPs were also tested through replicate experiments. The results showed a similar UV–vis peak when 0.25AuNP was synthesized in three replicates (Fig. 8a). For the stability test, the UV–vis spectra of the as-grown 0.25AuNP and after 45 weeks were evaluated, showing no difference (Fig. 8b). This indicates that AuNPs are stable over a long period of time and that the mango extract effectively capped the nanoparticles, preventing aggregation.

Fig. 8
figure 8

UV–vis spectra of 0.25AuNP (a) for three replicate synthesis and (b) right after synthesis and after 45 weeks.

This study reveals a simple, efficient, and eco-friendly synthesis of Gold Nanoparticles (AuNPs) mediated by a methanolic mango peel extract. The development of such energy- and resource-efficient synthesis protocols is crucial for maximizing the practical applications of nanoparticles for example in medical applications. The presented method offers distinct advantages over traditional chemical synthesis, known for its expense and environmental impact47, as well as microbial synthesis (using bacteria or fungi), which often requires complex and time-consuming processes (> 24 h)48,49.

Dyeing and characterization of cotton threads. Different colors of AuNP solution were produced by varying the initial concentration of gold ion used on its synthesis. The images of the synthesized AuNPs are presented in Fig. 9a. The AuNPs were used to dye cotton thread via the thermo-fixing method. As shown in Fig. 9b, the dyeing process successfully gives colors to the cotton threads.

Fig. 9
figure 9

(a) Synthesized AuNP (0.1, 0.25, 0.50, 0.75 and 1.0 consecutive figures from left to right) and (b) pristine cotton and corresponding dyed cotton threads with 0.1, 0.25, 0.50, 0.75 and 1.0 AuNP from left to right.

Scanning electron microscopy. Figure 10a presents the scanning electron microscopy (SEM) image of the pristine cotton, characterized by a clean surface with clearly discernible strands of cotton fiber. Notably, cotton samples dyed with 0.25AuNP displayed multiple grains on its surface which are highly likely the introduced gold nanoparticles as depicted in Fig. 10b. The image highlights the successful adherence of the AuNP to the cotton thread facilitated by the thermo-fixing method. The presence of AuNP to the cotton fabric was also validated by EDS. The spectra prominently displayed a mass percentage of 40% for gold, as shown in Fig. 10c. AuNP adhere to the surface of the cotton thread due to the fact that oxygen containing groups on the surface of the cotton, including hydroxyl and carboxylate groups combined with AuNP through complexing or electrostatic interaction50. This result is essential to ensure the integration of AuNP into the cotton fabric for the proper antibacterial functionalization of the fabric.

Fig. 10
figure 10

SEM micrograph of the (a) pristine cotton thread, (b) cotton dyed with 0.25AuNP and (c) EDS graph.

FTIR spectra of cotton. The broad peak at 3300 and 2895 cm-1 for the pristine cotton corresponds to the O–H stretching and C-H stretching due to cellulose macromolecules51 as shown in Fig. 11. The increase in the intensity of the corresponding peaks in the AuNP dyed cotton threads is due to the absorption of water and reductants52. The appearance of new peaks on the spectra of the AuNP dyed cotton fabrics at around 1650 and 1333 cm−1 correspond to N–H bending and O–H bending in phenol confirming the presence of AuNP synthesized by mango fruit peel extract on the cotton53.

Fig. 11
figure 11

FTIR spectra of the pristine cotton and the AuNP dyed cotton.

Color resistance to fade test. Different sets of cotton threads dyed with 0.10, 0.25, 0.50, 0.75 and 1.0AuNP were subjected to different harsh treatments with 1% acetic acid, 1% NaOH and detergent. Shown in Fig. 12 are the images of the AuNP dyed cotton samples, which exhibited good resistance to fade after being treated with 1% acetic acid, 1% NaOH and detergent with pH of about 10.5. All sets of AuNP dyed cotton samples retained their color after experiencing the given harsh treatments. This is due to the fact that AuNP exhibited a chemical bonding with the cotton threads as suggested in the FTIR spectra of the AuNP dyed cotton. AuNP probably exhibit complexing or electrostatic interaction with the cotton threads owing to their remarkable color resistance to fade54,55. These remarks highlights the excellent resistance to fading of the AuNP dyed cotton thread which is an important characteristic for various applications.

Fig. 12
figure 12

(a) AuNP dyed cotton, (b) AuNP dyed cotton treated with 1% acetic acid, (c) AuNP dyed cotton treated with 1% NaOH and (d) AuNP dyed cotton treated with detergent.

Antimicrobial activity. The antibacterial activity of pristine cotton and AuNP-dyed cotton fabrics was evaluated against the pathogenic microorganisms Staphylococcus aureus and Escherichia coli using the disk diffusion method. No zone of inhibition was observed for pristine cotton, whereas AuNP-dyed cotton exhibited inhibition against both S. aureus and E. coli. The corresponding zones of inhibition are presented in Table 2. These findings suggest the potential efficacy of AuNP-dyed cotton against Gram-positive bacteria like S. aureus and Gram-negative bacteria like E. coli. The antibacterial activity of the AuNP-dyed fabric varies depending on the type of bacteria, which may be attributed to differences in the cellular structures of Gram-positive and Gram-negative bacteria. For example, the distinct compositions of peptidoglycan and lipopolysaccharides in Gram-positive and Gram-negative bacteria have been reported to influence interactions between gold nanoparticles and biological surfaces56.

Table 2 Zones of inhibition (ZOIs) of AuNp dyed cotton threads, pristine cotton thread, and positive controls vs test microorganisms.

The antibacterial effect is likely due to the interaction of AuNPs present on the cotton surface with bacterial plasma membranes, cell wall proteins, and DNA through adsorption. The small size and surface chemistry of AuNPs enable them to penetrate bacterial membranes. The release of reactive oxygen species (ROS) by AuNPs during bacterial interaction can induce bacterial cell death through oxidative stress mechanisms57,58. The zone of inhibition for AuNP-dyed cotton against S. aureus is shown in Fig. 13. These results present the antibacterial efficacy of the AuNP-dyed cotton threads against Gram-positive and Gram-negative bacteria which could find various important applications in biomedical field to improve cotton gauze, face masks and other medical clothing.

Fig. 13
figure 13

Zone of inhibition of the AuNP dyed fabric against S. aureus.

This study presents a straightforward method for imparting color to cotton fabrics using gold nanoparticles (AuNPs), resulting in materials with high colorfastness and broad-spectrum antibacterial efficacy against Gram-positive and Gram-negative bacteria. Representing a considerable improvement over conventional nanoparticle integration methods that often involve harsh chemical reagents (e.g., NaOH, HNO3) 59and prolonged processing durations60, this technique utilizes a rapid thermo-fixation process. Efficient AuNP integration onto the cotton fabric was achieved, characterized by robust nanoparticle adhesion and potent antibacterial characteristics. While this investigation did not comprehensively assess the scalability or long-term environmental implications of the AuNP-dyed cotton fabric, these remain critical areas for subsequent research. Nevertheless, the functionalized cotton demonstrated notable resistance to fading under testing with NaOH, acetic acid, and detergent, highlighting the significant potential of AuNPs for scalable applications, including antibacterial textiles for the medical sector.

For possible health impact of AuNP dyed cotton thread, studies show the non-toxic effect of AuNP into normal cells. The work of Saqr et al. includes the report of the low toxicity of AuNP into primary osteoblast even at higher acceptable biological limit (20 µg/mL)61. Also, AuNP synthesized from Mentha longifolia leaf extract showed non-toxicity against human umbilical vein endothelial cells (HUVECs)62.

For the cost aspect of dyeing, 5 g of HAuCl4 from Merck is about 850 USD. This could produce 59 L of 0.25 mM gold ion solution. Fifty (50) ml of 0.25 mM AuNP could dye 100 inches of cotton thread, and so the approximate cost of dyeing per inch of cotton thread is approximately 0.00720 USD.

Conclusions

Gold nanoparticles (AuNPs) were successfully synthesized using a simple, eco-friendly method that utilized fruit peels of M. indica. UV–vis spectroscopy confirmed the presence of characteristic peaks of AuNPs, while DLS and TEM analyses revealed the presence AuNPs and their size distributions. Varying the initial concentration of gold ions during synthesis produced AuNP solutions in different shades of red, with deeper hues observed at higher concentrations. The synthesized AuNPs were effectively used to dye cotton threads through a heating process, imparting color with strong resistance to fading when exposed to acetic acid, NaOH, and detergent. This durability is likely attributed to the strong electrostatic interactions between the AuNPs and the cotton fibers during the dyeing process. Furthermore, the AuNP-dyed cotton exhibited significant antibacterial activity against both S. aureus and E. coli, demonstrating its potential for various fabric-based biomedical applications, such as antibacterial wound dressings, face masks, and protective clothing.