Open Access Article
Wahyu
Ramadhan†
ab,
Joko
Santoso†
a,
Uju
*ac,
Rahadiyan Garuda
Langit Dewangga
d,
Mario
Natanael
a,
Muhammad Aldy
Luthfiansyah
a,
Adinda Yulya
Rachmawati
ad and
Zacky Arivaie
Santosa
a
aDepartment of Aquatic Product Technology, Faculty of Fisheries and Marine Sciences, IPB University, Bogor 16680, Indonesia. E-mail: ujusadi@apps.ipb.ac.id
bCenter of Coastal and Marine Resources Studies (PKSPL), International Research Institute for Maritime, Ocean and Fisheries (i-MAR), IPB University, Bogor 16127, Indonesia
cSurfactant and Bioenergy Research Center (SBRC), IPB University, Bogor 16127, Indonesia
dPT IJO Inovasi Indonesia, Jl. Ciledug Raya No.125 B, Cipulir, Kebayoran Lama, Jakarta 12230, Indonesia
First published on 3rd October 2025
The demand for biodegradable straws has grown in response to environmental concerns regarding plastic waste. This study aimed to develop and optimize seaweed-based bioplastic straws with enhanced hydrophobicity, mechanical integrity, and biodegradability. Four base formulations combining agar, starch, carrageenan, and konjac were evaluated, with the B9 formulation (comprising agar and starch) selected as the most promising due to its superior thermal stability and low water absorption. This formulation was then used in a process optimization stage, where various homogenization parameters (speed, temperature, and time) were tested. The best-performing straw from this stage, referred to as low-speed-S-B9 (B9 processed under low-speed homogenization), demonstrated the most favorable overall performance, achieving a contact angle of 115.31 ± 1.15°, water absorption below 100.27 ± 2.67%, and tensile strength of 60.76 ± 2.78 MPa. SEM analysis revealed a dense and cohesive matrix structure, while FTIR spectra showed the main polysaccharide functional groups in all samples, with additional peaks reflecting each formulation's chemical composition. Thermal degradation profiles confirmed its heat resistance, with delayed onset and higher char residue. Mechanical and flexural tests showed the low-speed straw maintained high elongation and comparable bending resistance to commercial paper straws. Finally, soil burial testing confirmed full biodegradation of the straw within 60 days. These results confirm that low-speed homogenization of seaweed-based formulations offers a scalable and sustainable strategy to produce biodegradable straws with functional properties suitable for real-world use.
Sustainability spotlightOur research directly supports multiple United Nations Sustainable Development Goals (SDGs), particularly SDG 12 (Responsible Consumption and Production) and SDG 14 (Life Below Water). By valorizing seaweed—a renewable marine biomass—as the primary resource for bioplastic straws, we contribute to reducing reliance on fossil-based plastics and mitigating ocean plastic pollution, a critical threat to marine biodiversity. Furthermore, the development of biodegradable, thermally stable, and hydrophobic straws promotes sustainable material innovation for food-contact applications, minimizing waste and enhancing lifecycle sustainability. The use of low-speed homogenization for straw processing also supports SDG 9 (Industry, Innovation and Infrastructure) by offering an energy-efficient and scalable manufacturing route. Overall, this work integrates circular economy principles and marine biomass valorization, advancing environmentally responsible food packaging systems aligned with the global sustainability agenda. |
In response to this escalating crisis, governments and regulatory bodies worldwide have introduced stringent measures aimed at reducing plastic consumption through bans, financial incentives, and mandates for sustainable product design. This regulatory landscape, coupled with increased consumer awareness, has accelerated research into biodegradable and renewable alternatives that can effectively replace conventional plastics without sacrificing essential performance attributes.7–12 Among these products, disposable drinking straws, typically fabricated from polypropylene or polystyrene, have become a focal point due to their extensive usage, short lifecycle, and prominent role in environmental degradation.
Bioplastics derived from biomass such as cellulose, gelatin, and starch have attracted considerable interest. However, their widespread adoption remains hindered by critical limitations, notably poor thermal resistance, insufficient mechanical integrity, and high water affinity, which restrict their applicability, particularly in high-temperature, food-contact scenarios.13–15 Consequently, attention has increasingly shifted toward marine-derived biomass, particularly seaweed-based polysaccharides, as sustainable and scalable sources of high-performance biopolymer.16–19 Seaweeds like Gelidium and Gracilaria are especially promising owing to their rapid growth rates, high polysaccharide yields, and their inherent capability for atmospheric carbon sequestration during cultivation, making them strategically advantageous from both environmental and industrial perspectives.20,21 Moreover, the global movement towards utilizing seaweed-based polymers is gaining momentum due to their unique ability to significantly increase biomass productivity without requiring additional arable land or freshwater resources, thus avoiding competition with essential human food and agricultural needs.
Despite their sustainability credentials, seaweed-based biopolymers, particularly agar-based films, exhibit several performance deficits that critically limit their broader industrial and consumer acceptance. Agar films are inherently hydrophilic, possess inadequate mechanical strength, and exhibit limited thermal stability, thus constraining their practical use in applications that involve prolonged moisture exposure or elevated temperatures.22,23 Addressing these deficits necessitates innovative formulation strategies to enhance their functional properties while maintaining biodegradability and ensuring industrial scalability.
Polymer blending has been widely adopted as a strategic method to overcome natural limitations of single-component biopolymers. The integration of agar with other polysaccharides, such as carrageenan24,25 and corn starch,26,27 along with natural hydrophobic substances like beeswax,28 has been demonstrated to synergistically enhance mechanical integrity, thermal stability, and hydrophobicity. Additionally, the inclusion of inorganic fillers such as calcium carbonate (CaCO3) provides improved mechanical reinforcement and stability under thermal stress.29,30 Such composite approaches are essential for tailoring the physicochemical properties necessary to render seaweed-based bioplastic materials suitable for practical applications, particularly for food-contact packaging such as drinking straws. However, although various additives have been incorporated into agar-based matrices in previous studies, none has integrated all these components within a single formulation to comprehensively enhance performance, particularly in improving the hydrophobicity, heat resistance, and durability of agar-based biodegradable drinking straws.
Beyond compositional factors, the manufacturing process significantly influences the microstructural characteristics and resultant properties of bioplastics. Specifically, homogenization techniques, including mixing speed, temperature, and duration, critically determine the dispersion quality, interfacial adhesion, and morphological uniformity within polymer blends.14,31,32 Technically, high-shear homogenization (>10
000 rpm) has been the method of choice due to its effectiveness in achieving homogeneous dispersion at laboratory scale. However, its high energy consumption, scalability constraints, and operational complexity limit its practicality for industrial production. Conversely, low-speed homogenization methods (<10
000 rpm), such as overhead stirring, offer viable industrial alternatives with reduced energy demands and greater scalability potential, though their effectiveness in maintaining or enhancing bioplastic performance remains underexplored.
To bridge these critical gaps, this study systematically investigates the integrated effects of polymer blend composition and low-speed homogenization conditions on the development of biodegradable, hydrophobic, and heat-resistant seaweed-based bioplastic straws. Employing a factorial experimental design, the research evaluates the individual and combined impacts of polymer components (agar, carrageenan, corn starch, konjac, beeswax, CaCO3, citric acid) and optimized processing parameters (homogenization speed, temperature, and duration) on key functional attributes including surface hydrophobicity (contact angle), tensile properties, thermal degradation behavior, water absorption, and biodegradability. The outcomes of this research are expected to advance the development of sustainable bioplastic alternatives to petroleum-derived straws, supporting industrial feasibility, and contributing meaningfully to global efforts toward circular materials economies and sustainable resource management.
| Treat-ments | Agar (g) | Carra-geenan (g) | Corn starch (g) | Konjac (g) | Sorbitol (g) | Water (mL) |
|---|---|---|---|---|---|---|
| B1 | 2.5 | 2.5 | 0 | 2.5 | 50 | 150 |
| B2 | 6.0 | 0 | 0 | 1.5 | 50 | 150 |
| B3 | 5.0 | 2.5 | 0 | 0 | 50 | 150 |
| B4 | 2.5 | 2.5 | 5.35 | 2.5 | 50 | 150 |
| B5 | 6.0 | 0 | 5.35 | 1.5 | 50 | 150 |
| B6 | 5.0 | 2.5 | 5.35 | 0 | 50 | 150 |
| B7 | 7.5 | 0 | 0 | 0 | 50 | 150 |
| B8 | 5.0 | 2.5 | 0 | 0 | 50 | 150 |
| B9 | 7.5 | 0 | 5.35 | 0 | 50 | 150 |
| B10 | 5.0 | 2.5 | 5.35 | 1.5 | 50 | 150 |
In the first stage, each formulation was prepared by dispersing the dry ingredients into distilled water and heating to 90–95 °C under continuous stirring. The final slurry was homogenized using a high-shear homogenizer at 20
000 rpm for 5 minutes to ensure uniform dispersion. The mixture was then poured into flat glass trays and dried in a hot air oven at 50 °C for 6–7 hours. The resulting bioplastic films were demolded and characterized for water absorption and mechanical integrity. Based on these evaluations, four top-performing formulations were selected and coded as S-B1 to S-B10.
In the second stage, the selected film formulations were adapted for straw development. The straw formulation was enhanced by incorporating calcium carbonate (CaCO3), beeswax, and citric acid. Beeswax, calcium carbonate (CaCO3), and citric acid were incorporated to improve hydrophobicity, mechanical strength, and thermal resistance in straw form. The formulations used for straw production (the four top-performing bioplastic formulations) were incorporated with 9 g of calcium carbonate, 10 mL of beeswax, and 0.3 g of citric acid, based on previous reports by Chong et al.,33 Diyana et al.,34 and modified from Yoon et al..35 The preparation process followed the same thermal and mixing protocols. Beeswax was separately melted at 65 °C before being incorporated into the hot mixture, followed by citric acid and CaCO3. The final slurry was homogenized using a high-shear homogenizer at 20
000 rpm for 5 minutes to ensure uniform dispersion. The hot slurry was poured into cylindrical glass molds (2 cm inner diameter × 25 cm length) with an embedded stainless-steel rod (7 mm diameter) to form the inner cavity. Gelation was allowed at room temperature for 30 minutes before the samples were demolded and dried at 50 °C for 6 hours. The resulting straws were stored in desiccators prior to further analysis.
In the third stage, using one selected formula from stage 2, process optimization was conducted using low-speed overhead stirring as a potential alternative to high-shear mixing for industrial applications. A two-level factorial experimental design was employed, with three independent variables: temperature (60–80 °C), stirring speed (1500–2000 rpm), and mixing time (15–45 minutes). Eleven treatment combinations were executed, as presented in Tables 2 and 3. For each treatment, the same ingredient composition and casting protocol were used. Agar was first dissolved in distilled water at 90–95 °C, followed by the sequential addition of corn starch, carrageenan (if applicable), konjac (if applicable), sorbitol, beeswax (pre-melted), citric acid, and CaCO3 under continuous agitation. The resulting mixture was poured into the same cylindrical molds used previously.
| Parameter | Code | Low (−1) | Centre point (0) | High (+1) |
|---|---|---|---|---|
| Temperature (°C) | a | 60 | 70 | 80 |
| Time (minute) | b | 15 | 30 | 45 |
| Stirring speed (rpm) | c | 1500 | 1750 | 2000 |
| Run | Parameter | ||
|---|---|---|---|
| Temp. | Time | Speed | |
| a Information: low (L), center point (C), and high (H). | |||
| 1 | 70 (C) | 30 (C) | 1750 (C) |
| 2 | 70 (C) | 30 (C) | 1750 (C) |
| 3 | 80 (H) | 15 (L) | 1500 (L) |
| 4 | 60 (L) | 15 (L) | 1500 (L) |
| 5 | 60 (L) | 45 (H) | 1500 (L) |
| 6 | 70 (C) | 30 (C) | 1750 (C) |
| 7 | 60 (L) | 45 (H) | 2000 (H) |
| 8 | 60 (L) | 15 (L) | 2000 (H) |
| 9 | 80 (H) | 15 (L) | 2000 (H) |
| 10 | 80 (H) | 45 (H) | 2000 (H) |
| 11 | 80 (H) | 45 (H) | 1500 (L) |
Among the eleven trials, the best-performing treatment, based on appearance, water resistance, and structural properties, was identified and subjected to further characterization. This optimized straw was then compared against (i) the straw produced via high-shear homogenization and (ii) a commercial paper straw to evaluate the effects of mixing intensity on product performance, including biodegradability, mechanical properties, and industrial scalability.
In contrast, the lowest water absorption was found in B9 (52.73%), followed by B6 (67.94%), B10 (86.29%), and B5 (87.91%). In the context of straw applications, lower water absorption values are considered advantageous, as they indicate higher resistance to water penetration and better structural stability during use. These four formulations share key compositional traits: all contain corn starch, while B9 notably excludes carrageenan and konjac, suggesting that the presence of starch alone contributes significantly to reducing hydrophilicity by enhancing network density and reducing porosity.39 Both B6 and B10 contained carrageenan, while B10 additionally incorporated konjac. These formulations exhibited moderate water absorption, suggesting a complex interplay between the hydrophilic nature of carrageenan and konjac, which may be partially offset by the network-densifying effects of corn starch.
Formulations such as B1 (116.41%), B7 (123.62%), and B8 (125.92%) displayed intermediate water uptake, which could be attributed to their carrageenan content without sufficient balancing by starch or cross-linkers. On the other hand, B2 (99.06%), despite lacking carrageenan, still showed noticeable water uptake likely due to the presence of konjac, reaffirming its strong water-holding characteristics. These findings confirm that careful selection of biopolymer combinations is essential to achieving water-resistant films. Among the tested formulations, B9, which combined agar and corn starch with reinforcing additives (citric acid and CaCO3), offered the most desirable hydrophobic performance. Its superior dimensional stability and low water uptake justify its advancement to the next development phase.
While water absorption was determined in this study, the possible dissolution of low-molecular-weight additives such as sorbitol and citric acid during immersion was not directly quantified. No visible crystallization, whitening, or surface roughening was observed after drying, suggesting minimal migration of these components under the test conditions. Quantification of additive dissolution through chemical analysis of the immersion medium is recommended for future studies to better assess film stability.
Importantly, in this part, four film formulations—B5, B6, B9, and B10—exhibited the lowest water absorption values and were therefore selected for further processing into straw form. The selected candidates will be subjected to comprehensive evaluations in subsequent stages, focusing on thermal, mechanical, and biodegradation performance under optimized mixing conditions.
The FTIR spectra primarily reflected the characteristic functional groups of the constituent polymers and additives, as expected from a formulation prepared by physical blending. Subtle peak shifts and intensity variations were also observed, suggesting possible non-covalent interactions (e.g., hydrogen bonding, electrostatic, or hydrophobic effects) rather than new covalent bonds.
Fig. 2B reveals that all samples exhibited broad absorption peaks in the range of 3200–3400 cm−1, corresponding to O–H stretching vibrations, which are characteristic of hydroxyl groups in polysaccharides such as agar, carrageenan, and starch. Peaks observed around 2900 cm−1 correspond to the C–H stretching vibrations from aliphatic hydrocarbon chains in starch and agar. Notably, formulations B6 and B10, which contain carrageenan, demonstrated absorption bands near 1010–1080 cm−1, confirming the presence of sulphate ester (S
O) functional groups, characteristic of carrageenan, near 1010–1080 cm−1, confirming the presence of sulphate ester (S
O) functional groups, characteristic of carrageenan.40 These peaks were absent or less pronounced in B5 and B9, which did not include carrageenan, validating the spectral sensitivity to compositional differences.
Formulations S-B5 and S-B6, which include konjac flour, may also contribute unique spectral features. Although konjac's main component, glucomannan, shares similar polysaccharide backbones with agar and starch, it may introduce additional O–H and C–H vibrations due to its highly branched structure. However, its spectral fingerprint typically intersects with other hydrocolloids in the 3200–3400 cm−1 and 1000–1200 cm−1 regions. Therefore, while its presence may not be distinctly isolated in the FTIR spectra, it may still contribute to the overall hydrogen bonding within the matrix.
Further analysis showed the presence of characteristic bands near 1400–1500 cm−1, as well as distinctive peaks at 883 cm−1 and 708 cm−1, particularly in S-B6, S-B9, and S-B10, which confirm the successful incorporation of calcium carbonate (CaCO3) in the form of calcite polymorphs.41–43 These mineral-based bands were absent in the control films without CaCO3, supporting the structural modification introduced by the additive. In addition, the presence of C–O–C and C–O stretching vibrations was detected in the 1000–1200 cm−1 region, typical for polysaccharide backbones. Citric acid's role as a cross-linker may be reflected in slight band shifts and intensity changes in this region, consistent with previous reports at higher concentrations,44 although in the present formulation the evidence remains indirect.
While FTIR alone cannot conclusively identify these interactions, the observed spectral shifts may suggest contributions from hydrogen bonding among polysaccharides, electrostatic attraction between κ-carrageenan sulphate and Ca2+, and hydrophobic associations involving beeswax. These non-covalent effects are consistent with the improved water resistance and mechanical stability observed in Section 3.3.1. These interactions, while non-covalent, appear to synergistically improve both the mechanical integrity and water resistance of the straws.
Eventually, the FTIR profiles of the four formulations confirm the successful integration of their respective components and validate the formation of physically and chemically compatible biopolymer matrices. These spectral results support the compositional basis for the functional performance observed in water resistance and mechanical stability, highlighting the selection of S-B5, S-B6, S-B9, and S-B10 for further development into heat-resistant, hydrophobic bioplastic straws.
Surface wettability can be categorized based on contact angle values: 0° indicates super-hydrophilic surfaces, 0–90° hydrophilic, 90–120° hydrophobic, 120–150° ultra-hydrophobic, and values greater than 150° correspond to superhydrophobic materials.45 Based on this classification, S-B9 and S-B6 fall within the hydrophobic category, while S-B5 is closer to the hydrophilic threshold. The posthoc analysis conducted in this part confirmed that the differences in polymer composition, especially carrageenan content, had a significant effect (p < 0.05) on contact angle values.
These results align with the earlier FTIR findings, where the presence of sulphate ester (S
O) groups in carrageenan (present in S-B6 and S-B10) contributes to a more hydrophilic surface character. Although both starch and beeswax were included in all four samples and are known to influence surface energy, the differences in wettability are primarily attributed to the presence or absence of carrageenan and konjac. The lower contact angle of S-B5, for instance, is likely related to the hydrophilic behavior of konjac flour, which increases the matrix's water affinity.46
It is also important to note that the overall contact angle values (ranging from 85° to 114°) are considerably higher than those reported by Rhim,24 who observed contact angles of 46–56° for agar–carrageenan blends. This improvement is attributed to the presence of calcium carbonate and beeswax. Calcium carbonate has been shown to improve the hydrophobicity of seaweed-based bioplastics by reducing surface polarity,33 while beeswax enhances water resistance by lowering hygroscopicity and increasing the water barrier properties.39 In particular, S-B9, which contains neither carrageenan nor konjac, demonstrated the highest water repellency, supporting its potential as the most suitable formulation for applications requiring minimal water interaction. Similar observations were reported by Cunha and Grenha,47 who noted that carrageenan increases surface polarity and thus reduces hydrophobicity.
Overall, the enhanced hydrophobic behavior of B9 and B6 suggests their greater suitability for end-use scenarios involving prolonged contact with aqueous media, such as biodegradable drinking straws, where reduced surface wettability is essential to maintain structural integrity and user experience.
Formulations S-B6 and S-B9 exhibited the highest tensile strength values among the group. S-B6 achieved 93.35 MPa, while S-B9 followed with 73.33 ± 6.01 MPa. These values are substantially higher than those reported in previous agar-based bioplastic studies,21,48,49 indicating the structural reinforcing effect of calcium carbonate, starch, and beeswax. S-B6's superior strength can also be attributed to the controlled ratio of agar and carrageenan, with corn starch acting as a densifying filler that enhances network compactness.
In contrast, S-B5 and S-B10 displayed lower tensile strength values—44.40 MPa and 45.04 ± 1.92 MPa, respectively—suggesting that the presence of konjac or higher carrageenan content may compromise the polymer matrix uniformity. Konjac's water-binding nature can lead to microstructural inconsistencies, while excessive carrageenan disrupts agar's cohesive gel network.21,50 Elongation at break was significantly higher in formulations S-B5 (∼61%) and S-B10 (∼62.00), indicating enhanced flexibility attributed to the plasticizing effect of sorbitol and the structural contributions of konjac and carrageenan. In contrast, S-B6 (∼39%) and S-B9 (∼40) exhibited markedly lower elongation, suggesting increased stiffness and reduced extensibility in these biopolymer matrices.
These results illustrate a trade-off between tensile strength and elongation: S-B6 and S-B9 offered strong and rigid structures, ideal for maintaining straw integrity under stress, while S-B5 and S-B10 provided more elastic, flexible profiles. This balance between strength and flexibility is critical in tailoring bioplastic straw properties for consumer usability and durability during application. Overall, the findings validate the formulation strategies used in the development of S-B6 and S-B9 as strong candidates for durable bioplastic straws, while S-B5 and S-B10 may be optimized for scenarios where enhanced elasticity is desired.
Stage I (below ∼200 °C) reflected initial weight loss due to moisture evaporation. The S-B5 sample exhibited the highest weight reduction in this phase, likely due to its higher konjac content, a hydrocolloid known for its pronounced hygroscopicity. S-B10, which also contains konjac, showed moderate moisture loss, higher than S-B6 and S-B9 but lower than S-B5. This suggests partial hygroscopic behavior influenced by konjac concentration and matrix interaction.
Stage II (200–350 °C) was the primary degradation phase, during which polysaccharide chains underwent depolymerization and volatile components—including sorbitol, beeswax, and citric acid—were released. Among all samples, S-B9 exhibited the latest degradation onset and a relatively gradual decomposition profile, indicating greater matrix stability. This behavior is likely due to the combination of agar and starch without thermally labile hydrocolloids such as carrageenan or konjac. Moreover, the presence of calcium carbonate is thought to contribute to thermal shielding and char-promoting effects, enhancing the structural rigidity and stabilizing the degradation pathway.53
In contrast, S-B6 and S-B10, both containing carrageenan, showed slightly earlier thermal degradation onset and sharper mass loss slopes. This result is in line with the literature, where carrageenan's sulphated ester groups are thermally unstable and begin to decompose at lower temperatures than agar. S-B5, which includes konjac but no carrageenan, exhibited the most rapid and intense decomposition in this stage, reinforcing the thermolabile nature of glucomannan-based materials.
Stage III (>400 °C) corresponds to the breakdown of remaining carbonaceous structures and the formation of thermally stable residues. Here, S-B9 left the highest final residue (∼27%), followed by B10 (∼25.5%), S-B6 (∼24%), and S-B5 (∼22%). These residual trends are in agreement with microstructure (Fig. 6) and reflect the importance of both initial matrix composition and additive interactions in preserving structural coherence upon exposure to high temperatures. The incorporation of inorganic fillers like CaCO3 further contributed to residue formation by acting as a non-volatile matrix stabilizer and promoting carbonaceous char formation.
![]() | ||
| Fig. 6 SEM micrographs of selected bioplastic straw formulations (S-B5, S-B6, S-B9, and S-B10) at 500× and 2000× magnification. | ||
The DTG profiles revealed a clear differentiation in decomposition peaks. S-B9 displayed a sharp single degradation peak between 290–310 °C, while S-B6 and S-B10 showed broader or shoulder peaks, consistent with the overlapping thermal breakdown of carrageenan and other polymers. S-B5 and S-B10 both exhibited broadened DTG peaks with early shoulders around 260–280 °C, indicative of konjac's early decomposition. The overlap with carrageenan breakdown in S-B10 resulted in a slightly smeared double-peak profile, reflecting complex thermal interactions between these thermolabile polysaccharides.
Furthermore, DTA curves demonstrated the exothermic and endothermic nature of each decomposition phase. S-B9 exhibited the most defined endothermic peak at higher temperature ranges, suggesting more stable energy absorption prior to thermal collapse. B5 showed weaker and earlier DTA transitions, once again underlining its lower thermal integrity.
Among the samples, S-B9—formulated with 7.5 g agar and no carrageenan or konjac—exhibited the most cohesive and moderately compact matrix morphology. While some granular texture and surface unevenness were observed, the overall structure appeared more continuous and less porous compared to the other samples. This relatively uniform microstructure suggests favorable interpolymer compatibility and filler dispersion.
In contrast, S-B5, which incorporates 1.5 g konjac, presented a more porous and fibrous morphology. The surface was interspersed with irregular voids and microchannels, which can be attributed to konjac's strong hydrophilicity and swelling behavior during drying. Konjac's inclusion likely disrupted the uniform matrix formation, as its tendency to bind water and form gels can lead to localized phase expansion followed by collapse upon dehydration. This porous morphology may have facilitated greater water penetration, as supported by higher water absorption and elongation values in the physical tests. However, this structure could be beneficial in applications demanding flexibility or permeability.
S-B6, which replaces konjac with 2.5 g carrageenan, displayed more fractured and heterogeneous regions, including distinct microcracks and particle aggregation zones. These surface defects point to poor compatibility between carrageenan and starch in the presence of agar, possibly due to differences in charge distribution and polymeric chain interaction. The observed cracks and discontinuities indicate weak interfacial adhesion and inefficient plasticizer distribution, which may explain S-B6's relatively low elongation at break and moderate tensile strength.
Interestingly, S-B10 showed a heterogeneous yet slightly smoother surface compared to S-B6. Despite some irregularities, the combination of konjac and carrageenan may have improved interpolymer blending to a modest extent. However, notable surface granularity and unevenness remain, indicating that matrix integration was only partially achieved. These morphological features align with the intermediate mechanical and water barrier properties observed in S-B10.
Across all samples, residual calcium carbonate particles were occasionally visible, appearing as bright, unevenly distributed granules. These may have originated from partial sedimentation during casting or incomplete interaction with the polymer matrix. However, no visible trapped air bubbles or significant delamination were observed, indicating that the homogenization and degassing procedures during straw formation were effective. The beeswax, although not visually distinguishable in SEM, likely contributed to surface hydrophobicity and acted as a compatibilizer, improving the overall matrix integrity. Taken together, these microstructural observations corroborate the physicochemical trends previously discussed which were S-B9's structural compactness, S-B5's fibrous porosity, S-B6's phase separation, and B10's intermediate integration, demonstrating that component selection and blending strategy play a decisive role in determining the morphological and functional performance of biodegradable straw materials.
To further enhance its functional properties and production consistency, S-B9 was subjected to homogenization treatment using an overhead stirrer (characterized by lower speeds, <10
000 rpm) under varying speed and time conditions. A two-level factorial experimental design was employed, incorporating three independent variables: temperature (60–80 °C), stirring speed (1500–2000 rpm), and mixing time (15–45 minutes). Eleven treatment combinations were executed, as presented in Tables 3 and 4. The low-speed homogenization variant was referred to as low-speed S-B9, and the results of these optimization trials are presented in the following subsections.
| Parameters | Selected low-speed-S-B9 straw | High-speed-S-B9 straw | Commercial paper straw |
|---|---|---|---|
| a Note: values are expressed as mean ± standard deviation (n = 3). Different superscript letters (a–c) within the same row indicate significant differences at p < 0.05 (Tukey's HSD test). | |||
| Thickness (mm) | 0.67 ± 0.01a | 0.68 ± 0.01a | 0.56 ± 0.02b |
| Water absorption (%) | 100.27 ± 2.67a | 115.51 ± 2.83b | 120.1 ± 1.91c |
| Water solubility (%) | 5.20 ± 1.25a | 4.87 ± 0.40a | 8.35 ± 1.44b |
| Contact angle (°) | 115.31 ± 1.15a | 113.36 ± 3.98 ab | 103.12 ± 1.64c |
| Tensile strength (MPa) | 60.76 ± 2.78a | 73.33 ± 2.17b | 56.10 ± 2.63c |
| Elongation (%) | 34.61 ± 2.45a | 33.53 ± 2.85a | 11.95 ± 0.53b |
| Flexural strength (MPa) | 4.72 ± 2.09a | 4.61 ± 1.07a | 5.72 ± 0.18b |
Previously, the S-B9 formulation, while effective in producing hydrophobic and thermally resistant straws at the lab scale, relied on high-shear homogenization (>10
000 rpm). This posed practical limitations for industrial scaling due to high energy consumption, limited batch capacity, and operational safety concerns. To overcome this, a low-speed overhead homogenization strategy was implemented, aiming to preserve or improve product functionality while enhancing process feasibility.
A 32 factorial design was applied to evaluate the effects of homogenization speed (1500, 1750, and 2000 rpm), homogenization temperature (60–80 °C), and time (15, 30, 45 minutes) on straw performance. The matrix formulation was based on B9, previously identified as the most robust due to its compact microstructure, high contact angle, and thermal resilience. The optimization strategy aimed to maintain these characteristics under modified processing conditions. As shown in Fig. 7, water absorption values varied across treatment combinations. LLH recorded the lowest absorption in normal water (94.03 ± 0.64%), while LHL showed the highest (110.15 ± 6.08%). In hot water, HLL achieved the lowest absorption (100.27 ± 2.67%), while HHL reached 137.71 ± 2.23%.
Comparative analysis with high-speed homogenization revealed a notable improvement: the high-shear control sample absorbed up to 135.51 ± 2.83%, significantly higher than the best-performing low-speed straw (HLL). This suggests that gentle mixing supports more uniform CaCO3 and beeswax distribution, forming a denser matrix with fewer internal voids that typically promote water ingress. This effect aligns with prior findings that CaCO3 and lipid-based additives enhance water resistance by increasing matrix packing and reducing capillary diffusion paths.54 The HLL straw exhibited similar water absorption capacities in both normal water immersion (98.96 ± 1.93%) and hot water immersion (100.27 ± 2.67%). This finding supports its functionality for use in both cold and hot beverages and aligns with ISO 18188:2016 standards regarding straw resistance to extreme temperatures (both hot and cold). Altogether, the results confirm that low-speed overhead homogenization not only offers an energy-efficient, scalable alternative to high-shear processes, but can produce straws with comparable or superior water resistance. The HLL treatment, combining 80 °C, 15 minutes, and 1500 rpm, was identified as the most effective condition for future industrial application.
Compared with the commercial paper straw, the optimized low-speed-S-B9 straw showed ∼16.5% lower water absorption, a 12.3° higher contact angle, and nearly three times greater elongation, indicating improved water resistance and flexibility. Polylactic acid (PLA) straws, another widely promoted biodegradable alternative, can reach similar tensile strength but require high-temperature extrusion and degrade more slowly (>180 days) than the 60 days observed here. While the predicted production cost of the seaweed-based straw at a scaled-up level is still higher than PLA at present, the use of moderate processing temperatures (≤95 °C) and locally sourced seaweed offers potential for future cost reductions through process optimization and economies of scale.
The surface speckling observed on the selected low-speed S-B9 straw is attributed to suboptimal homogenization during the mixing process. The overhead stirrer employed in this study operates at low rotational speeds (1500–2000 rpm) and relies on high torque for material blending. It uses a direct current (DC) motor to drive the submerged rotor, enabling controlled shear mixing. This contrasts with the high-shear disperser homogenizer used by high-speed-S-B9 straw, which operates at speeds ranging from 10
000 to 20
000 rpm. These devices apply intense shear forces through a rotor–stator mechanism powered by motors up to 100 horsepower (hp), forcing fluid flow directly through the impeller axis.
Straws produced using the high-shear homogenizer demonstrated more uniform morphology compared to those processed with an overhead stirrer. The rotor–stator system subjects the medium to axial entry and radial discharge through a narrow gap between the rotor and stator, generating intense friction and particle size reduction. This process results in efficient dispersion and microstructural homogeneity. In contrast, overhead stirring promotes circular flow patterns, where the mixture cycles from the impeller down to the base and back upward, resulting in less intense mixing, while homogenizer flow is concentrated directly toward the rotor–stator axis.
The contact angle data provides further insight into surface hydrophobicity across the straw samples. Both the selected low-speed-S-B9 and high-speed-S-B9 straws exhibited similarly high contact angle values (113–115°), indicating no significant difference in their surface water repellency. In contrast, the commercial paper straw demonstrated a slightly lower contact angle (103°), placing it well below the hydrophobic performance of the bioplastic-based alternatives. The consistently higher hydrophobicity of both bioplastic straws, relative to the commercial control, reinforces their potential for superior resistance to wetting and prolonged structural integrity in moist environments. This increase was likely due to more stable surface structuring, calcium carbonate and wax distribution, as high-speed shear may disrupt the polar–nonpolar interface, reducing surface repellence. Following Bracco and Holst,56 surfaces with contact angles between 90° and 120° are considered hydrophobic, while those above 120° are classified as ultra-hydrophobic. Importantly, the lower-speed process achieved a level of quality comparable to, or even exceeding, that of the high-speed and commercial products, particularly within the hydrophobicity range typical of coated paper straws. Additionally, visual inspection in Fig. 9 showed that after 4 hours of soaking, both the selected low-speed-S-B9 and high-speed-S-B9 straws maintained their shape and structural integrity equally well, in contrast to the commercial straw, which exhibited noticeable deformation. This visual evidence supports the quantitative data and highlights the superior moisture resistance of the bioplastic formulations compared to the paper-based control.
In terms of elongation, the selected low-speed-S-B9 and high-speed-S-B9 straws performed similarly, with values of 34.61% and 33.53%, respectively. Both formulations exhibited substantially greater ductility than the commercial straw (11.95%), indicating better flexibility and energy absorption under stress—key attributes of straw for everyday usability. Flexural strength showed no substantial difference among the samples. The commercial paper straw recorded a value of 5.72 MPa, which was comparable to the selected low-speed-S-B9 (4.72 MPa) and high-speed-S-B9 (4.61 MPa). Despite slight numerical variation, all three straws demonstrated similar bending resistance (Fig. 8f).
Visual inspection and structural analysis revealed distinct degradation patterns. On day 0, all straws retained full structural integrity. By day 20, the low-speed and high-shear straws began to exhibit signs of surface erosion and small cavities, while the paper straw displayed discoloration and early signs of delamination. By day 40, the bioplastic straws showed significant breakdown with large areas of fragmentation, and the paper straw had become highly brittle. On day 60, both bioplastic straw types were fully degraded and no longer identifiable in the soil, whereas remnants of the paper straw were still observable. These findings align with prior reports indicating that starch-based bioplastics are highly susceptible to microbial degradation in moist and aerated environments.58 The presence of polysaccharides such as agar and starch, coupled with biodegradable plasticizers and fillers, enhances microbial enzymatic activity, promoting complete material breakdown. Notably, the similar degradation profiles between low-speed and high-shear straws further affirm that the process optimization did not impair the material's composability. The observed biodegradation performance confirms the environmental viability of the developed seaweed derived straws and supports their application as a sustainable alternative to synthetic polymer-based single-use straws.
Footnote |
| † WR and JS equally contributed to this work and share common first authorship. |
| This journal is © The Royal Society of Chemistry 2025 |