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Investigation on the interactions between amphiphilic copolymer and different surfactants

  • Yun Zhang

    Yun Zhang: PhD candidate in Jiangnan University, major in chemical engineering and technology. His research interests include macromolecular self-assembly, surfactants and daily chemical.

         , Sihan Yu

    Sihan Yu: intermediate engineer, she received master degree from East China University of Science and Technology in 2018, major in Physical Chemistry. She is mainly engaged in the cosmetic research.

         , Hao Du

    Hao Du: postgraduate, he is studying chemical engineering with a focus on amphiphilic polymer, surfactant, bijel and Pickering emulsion.

         , Yuhua Cao

    Yuhua Cao: professor, she received Ph.D. degree from East China Normal University in 2002, major in analytical chemistry. Her reseach interests include amphiphlic random copolymer, surfactants, and photonic crystal.

     EMAIL logo     , Hujun Xu

    Hujun Xu: professor, he received his Ph.D. degree in 2005 from Nanjing University of Science and Technology, P.R. China. He has been involved in surfactants and detergents for over 30 years. He has published over 70 papers in the field of surfactants and detergents.

         and Jie Shen
Published/Copyright: October 21, 2025
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Tenside Surfactants Detergents
From the journal Tenside Surfactants Detergents Volume 62 Issue 6

Abstract

As a newly developed amphiphilic copolymer, poly (N-vinylpyrrolidone-co-methacrylic acid) (P(NVP-co-MAA)) has excellent lubricity and can be potentially employed in household detergents, personal cleaning and care. In this study, the interactions between P(NVP-co-MAA) and five different surfactants were investigated using the surface tension method. The results show that P(NVP-co-MAA) can interact with the two anionic surfactants which respectively contain COO− and SO3 2− groups. In contrast, P(NVP-co-MAA) can’t interact with zwitterionic and cationic surfactants. The further study indicates that the electrostatic attraction between P(NVP-co-MAA) and the anionic surfactants benefits the formation of the mixed aggregation. However, as the surfactants contain quaternary ammonium groups, the electrostatic repulsion, steric hindrance and high interaction energy may hinder the binding of P(NVP-co-MAA) and these surfactants. Finally, the effect of NaCl on P(NVP-co-MAA)-anionic surfactant mixtures was studied. In the case that the surfactant has the SO3 2−group, the addition of NaCl at the concentration not exceeding 0.5 g L−1 helps the formation of P(NVP-co-MAA)- surfactant aggregation. However, when the hydrophilic group of the surfactant is substituted by the COO− group, the addition of NaCl regardless of concentration inhibits the interaction of P(NVP-co-MAA) and the surfactants. This study offers a new guideline to select appropriate surfactants for P(NVP-co-MAA)-containing formulations.

Keywords: amphiphilic copolymer; surfactant; interaction

1 Introduction

Poly (N-vinylpyrrolidone-co-methacrylic acid) (P(NVP-co-MAA)) is a type of amphiphilic random copolymer with both hydrophobic (NVP) and hydrophilic (MAA) monomer units. 1 , 2 , 3 , 4 , 5 The sequence distribution of the monomer units in the polymer chain is random, resulting in the ill-defined chain structure. However, the synthesis of such copolymers is facile and cost-effective, which is suitable for industrial preparation. Thus, it is meaningful to explore the application of this copolymer. Because of the amphiphilic structure, P(NVP-co-MAA) has excellent properties such as solubility and emulsification, making it potentially applied in emulsifier, micellar nanoreactor and slow-release agent. In particular, it is found that the N-vinylpyrrolidone (NVP) group of P(NVP-co-MAA) can be adsorbed on the surface of hair, thereby increasing hair lubricity. As a result, P(NVP-co-MAA) can be served as a substitute for silicone oil. 6 In addition, methacrylic acid (MAA) can also improve lubricity by effectively reducing abrasion. 7 Thus, P(NVP-co-MAA) is considered as a promising candidate in surfactant-based household detergent and personal care formulations. In addition, understanding the interactions between P(NVP-co-MAA) and surfactants is beneficial to explore high-performance formulations that satisfy consumers’ increasing demands.

Interactions of surfactant-containing systems have been a research hotspot for many years. 8 , 9 , 10 , 11 It is an interesting phenomenon that the mixtures comprising two or more different components exhibit superior interfacial and colloidal performance than their individual ones, such as lower surface tension, more satisfying emulsification and foaming properties. 12 , 13 Besides increasing the surface chemical properties, the interaction can also reduce the amount of each component, thereby lowing costs and improving efficiency. Nowadays, many researchers focus on the interactions between different common surfactants, such as nonionic/nonionic, 14 ionic/nonionic 15 and zwitterionic/ionic 16 , 17 surfactants. It is suggested that stronger interactions between surfactants contribute to greater synergistic effects. 8 Accordingly, synergistic interactions within cationic/anionic surfactant systems are often considered as most effective ones due to strong electrostatic interactions between oppositely charged headgroups.

With the advanced development of innovative functional polymers, more and more surfactant-based formulations containing these polymers have remarkable efficacy. Subsequently, the interactions between polymers and surfactants have been received great interest. In a polymer-surfactant complex, the interactions include electrostatic attraction, hydrogen bonding, hydrophobic and diploe interaction. 18 , 19 , 20 , 21 The further study shows that the interactions depend on the different types of surfactants and polymers. It is in good agreement that hydrophobic interaction mainly occurs in neutral polymer-surfactant complex while electrostatic interaction is dominant in polymer-surfactant mixture with opposite charge. Wang et al. 22 investigated the interactions between polymers and anionic/nonionic surfactants. The results show that the hydrophobic interaction leads to the formation of mixed adsorption layer in oil and water surface, achieving ultra-low interfacial tension. Lei et al. 23 studied the interactions between an esterified amide gemini surfactant and a non-ionic polymer – polyvinylpyrrolidone (PVP). The study suggests that the aggregates are formed through electrostatic interaction because PVP is easy to be protonated. 24 , 25 Although interactions between polymers and surfactants have been investigated, the interactions of a specific polymer and different types of surfactants are rarely reported. In practice, functional polymers need to be added in surfactant-containing formulations to exert their distinctive properties. 26 , 27 Therefore, it is essential to select appropriate surfactants that can interact with the polymers. Meanwhile, understanding the interactions between different types of surfactants and a particular polymer provide critical theoretical guidelines for rational design of surfactant and polymer-containing formulation.

In this study, the interactions between P(NVP-co-MAA) and five different surfactants (Figure 1) were investigated using the surface tension method. Considering that P(NVP-co-MAA) is potentially applied in household detergents and personal cleaning and care, the selected surfactants are commonly used in these formulations. The surfactants include two anionic surfactants (sodium lauroyl sarcosinate (SLS) and sodium dodecyl sulfonate (SDS)), two zwitterionic surfactants (laurylamide propyl betaine (LAB) and laurylamide propyl hydroxysulfobetaine (LHSB)), and one cationic surfactant (Dodecyl trimethyl ammonium bromide (DTAB)). The interactions between P(NVP-co-MAA) and the surfactants were investigated by the surface tension versus concentration curves. In addition, the detailed interaction mechanisms were also explained in this study.

Figure 1: Structures of P(NVP-co-MAA) and five surfactants.
Figure 1:

Structures of P(NVP-co-MAA) and five surfactants.

2 Experiments

2.1 Materials

P(NVP-co-MAA) with a molecular weight of 11,500 Da was prepared in our lab. 1 The molar ratio of NVP and MAA is 6:4. The Polymer Dispersity Index (PDI) is 1.84. The detailed information of P(NVP-co-MAA) are shown in Figure S1-S3 in Supplementary Material. Sodium lauroyl sarcosinate (SLS, CAS: 137-16-6; substance content: 30 %) was obtained from Fengyi Co.,Ltd., sodium dodecyl sulfonate (SDS, CAS: 2,386-53-0; substance content: 37 %) was purchased from Meryer (Shanghai) Chemical Technology Co., Ltd., laurylamide propyl betaine (LAB, CAS: 61,789-40-0; substance content: 35 %) was gained from Guangzhou Tinci Materials Technology Co., Ltd., laurylamide propyl hydroxysulfobetaine (LHSB, CAS: 13,197-76-7; substance content: 35 %) was obtained from Shandong Usolf Chemical Technology Co., Ltd., dodecyl trimethyl ammonium bromide (DTAB, CAS:1119-94-4; substance content: 50 %) were purchased from Jinan Fine industry & Trade Co., Ltd. The characteristic properties of the surfactants are listed in Table S1 in Supplementary Material. All the deionized water used in this experiment was obtained from a Millipore purification system.

2.2 Measurement of surface tension

The surface tension was measured by the Wilhelmy Plate method 28 via a BZY-3B surface tension meter (Ping xuan Technology Instrument Co., Ltd., Shanghai, China). The temperature was set at 25 °C during the whole experiment. Before every measurement, the platinum plate was firstly washed by ultrapure water and then was burned red by alcohol lamp to keep absolutely clean. After cooling down, the platinum plate was put into the sample cell and the measurement was performed by starting the instrument. In this experiment, the concentration of P(NVP-co-MAA) was ranged from 0 to 0.8 g L−1, meanwhile, the concentrations of the five surfactants were respectively 0.1–10 g L−1 for SLS and SDS, 0.01–10 g L−1 for LHSB, 10−4 to 10 g L−1 for DTAB. The instrument was calibrated using deionized water with the value of surface tension of 72 ± 1.0 mN m−1 before experiment. Each sample was measured by a mean average of three readings at an interval of 30 s. All the samples in this study were measured in triplicate. Finally, the surface tension versus concentration curves were plotted according to the values from the measurements.

3 Results and discussion

3.1 Interactions between P(NVP-co-MAA) and anionic surfactants

The two anionic surfactants (SLS, SDS) were respectively mixed with P(NVP-co-MAA). The corresponding γ-logcs curves are shown in Figures 2 and 3. Considering that P(NVP-co-MAA)-surfactant system will be applied in practical shampoo formulations, the pH was adjusted to 7. As P(NVP-co-MAA) with different concentrations is respectively added into the two surfactant solutions, the “three inflection points corresponding to two plateaus” feature 29 appears in all the curves. These curves are explained as follows:

Figure 2: The surface tension curves of P(NVP-co-MAA)/SLS mixed system at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).
Figure 2:

The surface tension curves of P(NVP-co-MAA)/SLS mixed system at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).

Figure 3: The surface tension curves of P(NVP-co-MAA)/SDS mixed system at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).
Figure 3:

The surface tension curves of P(NVP-co-MAA)/SDS mixed system at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).

Initially, the surface tension of the complex decreases with the concentration of the anionic surfactant increasing. The polymer-surfactant complex exhibits a lower surface tension than the single surfactant at the same concentration. This phenomenon may be explained that P(NVP-co-MAA) has the ability to reduce intermolecular electrostatic repulsion in anionic surfactant molecules, improving their adsorption at the interface and thus reducing surface tension. 29 It is also suggested that P(NVP-co-MAA) may participate in the surface adsorption, thus effectively help the surface tension decrease. 22 As the surface tension declines to the first inflection point, the anionic surfactant and P(NVP-co-MAA) begin to interact with each other. Accordingly, the critical aggregation concentration (cac) is obtained, implying the initial aggregation of P(NVP-co-MAA) and surfactant. 25 Then the surface tension of the complex maintains a stable plateau until the emergence of the second inflection point, corresponding to saturated binding concentration (c0). It is also implied that c0 represents the saturation adsorption of the surfactant onto P(NVP-co-MAA). 30 , 31

From cac to c0, more and more surfactant molecules are adsorbed by P(NVP-co-MAA) molecules, leading to the presence of first plateau of surface tension. In this process, the surfactant interacts with P(NVP-co-MAA) to form mixed aggregates. Up to now, there exists two kinds of configuration modes to describe the interaction between polymers and surfactant. One is the “beads-on -a string” mode. 32 , 33 The other is the “necklace” mode. 24 , 34 The former suggests that the polymer chains pass through the centers of every micelle of surfactants. The latter argues that the aggregated surfactant molecules are surrounded by P(NVP-co-MAA) molecules. To further illustrate the interaction between P(NVP-co-MAA) and the anionic surfactants, the interaction forces were discussed in this study. It is clear that the nitrogen atoms of amide groups and oxygen atoms of carbonyl groups in NVP monomer units are easily protonated in aqueous solution at pH seven and become positively charged. Thus, the protonated NVP monomer units are favorable to interact with COO− groups of anionic surfactants through electrostatic attraction. It seems that the COO− groups also exist in MAA monomer units and would repulse the anionic surfactant due to the same charge. However, the result is opposite, showing that this electrostatic repulsion is weaker than the electrostatic attraction. In addition, the molar ratio of the monomer unit of NVP is higher than that of MAA in this employed P(NVP-co-MAA). Therefore, the electrostatic attraction is dominant in this polymer-surfactant system. This result is in good agreement in the previous literature that the molar ratio of monomer units in polymer has an significant effect on the interaction between polymer-surfactant system. 4 In addition, the hydrophobic interaction occurs between the hydrocarbon chains of both P(NVP-co-MAA) and the anionic surfactant. 24 Thus, it can be inferred that both electrostatic and hydrophobic interactions have significant effects on the binding of P(NVP-co-MAA) to anionic surfactants.

As seen in Figures 2 and 3, when the anionic surfactant concentration exceeds c0, the surface tension continues decreasing to the third inflection point, which corresponds to the critical micelle concentration (cmce). 35 , 36 It can be illustrated that the P(NVP-co-MAA) molecules no longer adsorb the anionic surfactant molecules because of saturation adsorption. As a result, excess surfactants are adsorbed in the interface of the mixture, leading to the surface tension further dropping. The emergence of cmce indicates the saturation adsorption of free anionic surfactants, accompanied with the formation of micelles.

The surface tension and critical micelle concentration (cmc of SLS at 25 °C are 43.50 mN m−1 and 2.29 g L−1, respectively (Figure 2). As the concentration of P(NVP-co-MAA) increases from 0.05 to 0.8 g L−1, the value of cac increases slightly, but it is still lower than that of cmc (Table 1). Meanwhile, the value of γcac decreases from 59.29 to 55.22 mN m−1. This implies that the interaction of P(NVP-co-MAA) and SLS results in the surface activity improving. In addition, the cac value is much lower than the cmce value at any P(NVP-co-MAA) concentration. It is also revealed that the mixed aggregations above are more stable than the single surfactant micelles. As the P(NVP-co-MAA) concentration continuously increases, the plateau ranging from cac to c0 steadily extends. The reason can be explained that more P(NVP-co-MAA) molecules induce more SLS molecules to interact with them, making the system more stable. As shown in Figure 3, the surface tension and cmc of single SDS are 28.77 mN m−1 and 4.01 g L−1, respectively. When the concentration of P(NVP-co-MAA) rises to 0.8 g L−1, the cac value of the mixed aggregation reaches 0.69 g L−1, much lower than the cmc value of SDS alone. It is shown that adding P(NVP-co-MAA) in SDS solution has a positive effect on the interfacial properties. Moreover, the value of cac is smaller than that of cmce in every curve in Figure 3. Furthermore, the plateau in the range of cac to c0 becomes widen as the concentration of P(NVP-co-MAA) increases. These results are in consistent with that in P(NVP-co-MAA)-SLS system. It is also indicated that the interaction between P(NVP-co-MAA) and SDS benefits to form more stable mixed aggregation, providing satisfied interfacial properties. Thus, it can be concluded that the combination of the anionic surfactant (SLS or SDS) and P(NVP-co-MAA) not only reduces the consumption of each individual component, but also improves the surface activity. These mixtures have great potential in formulation application.

Table 1:

Surface chemical property parameters of P(NVP-co-MAA)/SLS mixed system at 25 °C.

cP(NVP-co-MAA) (g L−1) cac (g L−1) γcac (mN m−1) c0 (g L−1) γc0 (mN m−1) cmce (g L−1) γcmce (mN m−1)
0.05 0.40 59.29 0.79 57.85 2.24 42.87
0.1 0.44 58.10 0.91 57.37 2.30 42.99
0.4 0.51 56.14 1.11 55.06 2.34 43.06
0.8 0.54 55.22 1.36 54.37 2.51 43.13
Table 2:

Surface chemical property parameters of P(NVP-co-MAA)/SDS mixed system at 25 °C.

cP(NVP-co-MAA) (g L−1) cac (g L−1) γcac (mN m−1) c0 (g L−1) γc0 (mN m−1) cmce (g L−1) γcmce (mN m−1)
0.05 0.61 56.39 0.86 56.03 4.15 28.49
0.1 0.63 54.85 1.01 54.48 4.20 28.50
0.4 0.67 51.32 1.23 51.02 4.34 28.56
0.8 0.69 49.84 1.74 49.69 4.79 28.70

To further investigate the effect of hydrophilic groups (COO−, SO3 2−) on the interaction of the P(NVP-co-MAA)-anionic surfactant system, SLS and SDS were selected considering that they have the same carbon chains (C12). Compared with Figure 2, Table 1 and Figure 3, Table 2, it is not difficult to find that the first plateau in P(NVP-co-MAA)-SDS system is broadener than that in P(NVP-co-MAA) -SLS system. The difference may be attributed to the diverse charges of head groups. Yan et al. 37 investigated the interactions of polyvinyl alcohol (PVA) with two surfactants, which contained SO3 2− and–OSO3 2- groups, respectively. It is found that the surfactant with–OSO3 2−group interacts with PVA more intensely than that with SO3 2−group due to the higher negative charge. It is well known that the SO3 2− group is more electro-negative than the COO− group, thus it has a greater tendency to interact with the easily protonated P(NVP-co-MAA) through electrostatic attraction Table 3.

Table 3:

Surface chemical property parameters of P(NVP-co-MAA)/LAB mixed system at 25 °C.

cP(NVP-co-MAA) (g L−1) cmce (g L−1) γcmce (mN m−1)
0.05 0.36 33.06
0.1 0.37 32.64
0.4 0.40 32.59
0.8 0.38 32.58

3.2 Interactions between P(NVP-co-MAA) and zwitterionic surfactants

Zwitterionic surfactants have excellent properties such as electric resistance, lubrication. They play an important role in household detergents, as well as personal cleaning and care. To better develop P(NVP-co-MAA)-containing formulations, it is necessary to understand the interactions between P(NVP-co-MAA) and zwitterionic surfactants. As discussed above, the anionic surfactants containing the COO− or SO3 2− group can interact with P(NVP-co-MAA). Accordingly, to further investigate the interactions between P(NVP-co-MAA) and zwitterionic surfactants containing the COO− or SO3 2− group, lauramidopropyl betaine (LAB) and lauramidopropyl hydroxysulfobetaine (LHSB) were selected to complex with P(NVP-co-MAA). To eliminate extra interferences, all the surfactants involved in this study have the same carbon chain length (C12).

Figure 4 shows the γ-logc curves of the mixture of P(NVP-co-MAA) and LAB. The surface tension and cmc of LAB are respectively 32.90 mN m−1 and 0.41 g L−1. As the concentration of P(NVP-co-MAA) ranges from 0.05 to 0.8 g L−1, the γ-logc curves of the mixture almost overlap. In addition, from Figure 4 and Table 3 the “three inflection points corresponding to two plateaus” feature can’t be found in P(NVP-co-MAA)-LAB system. It is implied that there is no apparent interaction between LAB and P(NVP-co-MAA). Although LAB and SLS have the same COO− group and hydrophobic chain length, P(NVP-co-MAA) only can interact with SLS rather than LAB. Detailed analysis based on the structures of LAB and SLS shows that the quaternary ammonium group of LAB may hinder interaction with P(NVP-co-MAA). It is known that the quaternary ammonium group of LAB is positively charged. On the other hand, the NVP monomer units in P(NVP-co-MAA) are also positive due to the protonation of the N and O atoms respectively in the amide and carbonyl groups. Therefore, there exists electrostatic repulsion that inhibits the binding of P(NVP-co-MAA) and LAB. In addition, the protonated quaternary ammonium group is so large that it hinders the interaction between P(NVP-co-MAA) and LAB due to spatial hindrance. Although the COO− group in LAB can generate the electrostatic attraction toward the protonated NVP monomer units in P(NVP-co-MAA), the result suggests that this electrostatic attraction is weak and is offset by the strong electrostatic repulsion. Since there are more NVP monomer units than MAA monomer units in P(NVP-co-MAA) in this study, the polymer-chain of P(NVP-co-MAA) have more positive charges. Thus, as P(NVP-co-MAA) is close to LAB, the electrostatic repulsion is dominant. In addition, the spatial hindrance also inhibits the binding of LAB and P(NVP-co-MAA).

Figure 4: The surface tension curves of P(NVP-co-MAA)/LAB mixed system at 25 °C (cmce represents critical micelle concentration).
Figure 4:

The surface tension curves of P(NVP-co-MAA)/LAB mixed system at 25 °C (cmce represents critical micelle concentration).

Figure 5 presents the γ-logc curves of P(NVP-co-MAA) and LHSB system. It is found that the γcmce nearly keeps constant as the concentration of P(NVP-co-MAA) rises from 0 to 0.8 g L−1 (Table 4), suggesting that P(NVP-co-MAA) has no effects on LHSB adsorption at the interface. In addition, P(NVP-co-MAA) and LHSB cannot aggregate together to form mixed system since there are no any inflection points in the curves even though LHSB contains SO3 2−group. Thus, it can be inferred that the quaternary ammonium group, which is served as the cationic component of LHSB, is not beneficial to the combination of P(NVP-co-MAA) with LHSB.

Figure 5: The surface tension curves of P(NVP-co-MAA)/LHSB mixed system at 25 °C (cmce represents critical micelle concentration).
Figure 5:

The surface tension curves of P(NVP-co-MAA)/LHSB mixed system at 25 °C (cmce represents critical micelle concentration).

Table 4:

Surface chemical property parameters of P(NVP-co-MAA)/LHSB mixed system at 25 °C.

cP(NVP-co-MAA) (g L−1) cmce (g L−1) γcmce (mN m−1)
0.05 0.59 37.06
0.1 0.58 37.18
0.4 0.59 37.02
0.8 0.47 37.21

3.3 Interactions between P(NVP-co-MAA) and cationic surfactants

As discussed above, P(NVP-co-MAA) can interact with anionic surfactants containing the COO− or SO3 2− group. These polymer-surfactant mixtures are prone to form aggregations that effectively improve the surface properties. However, as the zwitterionic surfactant that has quaternary ammonium group and COO− or SO3 2− group, the interaction between the polymer and surfactant disappears. To further confirm the effect of the quaternary ammonium group on the interactions in P(NVP-co-MAA)-containing mixtures, the cationic surfactant dodecyltrimethylammonium bromide (DTAB), which has only one quaternary ammonium group was selected in this study. As seen in Figure 6 and Table 5, the characteristic “three inflection points corresponding to two plateaus” feature is absent in all curves with the concentration of DTAB ranging from 0 to 0.8 g L−1. It is suggested that P(NVP-co-MAA) can’t interact with DTAB. Combined with the result from P(NVP-co-MAA)- zwitterionic surfactants system, it is further confirmed that the presence of the quaternary ammonium group has negative effects on the binding of P(NVP-co-MAA) and surfactants. It seems that the MAA monomer units in P(NVP-co-MAA) have COO− groups that can interact with cationic surfactant via electrostatic attraction. However, as mentioned above, the number of NVP monomer units is more than that of MAA in the P(NVP-co-MAA) molecules discussed, thus the NVP monomer units are dominant. Since the NVP monomer units are easy to be protonated due to the existence of amide groups and carbonyl groups, the strong electrostatic repulsion between P(NVP-co-MAA) and DTAB inhibits the interaction with each other. Besides, it is proposed that the introduction of quaternary ammonium group makes the cationic surfactants own larger head group than anionic surfactants, it is difficult to interact with polymers because of steric hindrance. 38 Furthermore, it agrees well that the interaction between polymer and cationic surfactant needs high energy, resulting in the complex unstable. 13 Therefore, P(NVP-co-MAA) and DTAB can’t interact with each other ascribed to electrostatic repulsion, steric hindrance and high interaction energy.

Figure 6: The surface tension curves of P(NVP-co-MAA)/DTAB mixed system at 25 °C (cmce represents critical micelle concentration).
Figure 6:

The surface tension curves of P(NVP-co-MAA)/DTAB mixed system at 25 °C (cmce represents critical micelle concentration).

Table 5:

Surface chemical property parameters of P(NVP-co-MAA)/DTAB mixed system at 25 °C.

cP(NVP-co-MAA) (g L−1) cmce (g L−1) γcmce (mN m−1)
0.05 0.25 37.72
0.1 0.27 37.71
0.4 0.32 37.68
0.8 0.31 37.85

3.4 Effects of NaCl on interactions between P(NVP-co-MAA) and anionic surfactants

It is known that adding electrolytes can change surfactant properties such as surface tension and cmc, especially for ionic surfactants. Ions from electrolytes can adsorb counterions from surfactants through electrostatic attraction, reducing the electrostatic repulsion among surfactants. 39 This makes surfactants more likely to aggregate into micelles. Although the effects of electrolytes on individual surfactants have been deeply investigated, the effects of electrolytes on surfactant-polymer systems are rarely reported. In this study, NaCl was chosen to investigate the influence of electrolyte on the mixture of P(NVP-co-MAA) and anionic surfactant (SLS or SDS).

Figure S4 shows the curves of surface tension versus concentration of NaCl. the P(NVP-co-MAA) concentration was fixed at 0.05 g L−1, while the concentration of NaCl varied from 0.5 to 2 g L−1. The concentrations of SLS were selected from 0.1 to 10 g L−1, including cac (0.4 g L−1), c0 (0.8 g L−1) and cmce (2 g L−1). The surface tension of the complex decreases as the concentration of SLS increases. It is suggested that SLS effectively improves the surface property of the mixed system. In addition, as the concentration of NaCl increases, the surface tension also decreases. This situation is the same as in the individual surfactant system. It can be explained that Na+ interacts with the COO− group of SLS, lessening the electrostatic repulsion among SLS molecules in the mixture system. At the same time, the surface tensions from cac to c0 are similar when the NaCl concentration reaches 0.5 g L−1, implying the presence of a clear plateau. As the NaCl concentration keeps increasing, the difference of surface tensions from cac to c0 are distinctive, indicating the disappearance of plateau. This result is in good agreement in the data presented in Figure 7 that the “three inflection points corresponding to two plateaus” feature only exists as the NaCl concentration is 0.5 g L−1.

Figure 7: The surface tension curves of 0.05 g L−1 P(NVP-co-MAA)/SLS mixed system with different concentrations of NaCl at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).
Figure 7:

The surface tension curves of 0.05 g L−1 P(NVP-co-MAA)/SLS mixed system with different concentrations of NaCl at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).

As seen from Table 6, in the absence of NaCl, the values of cac and c0 are respectively 0.40 and 0.79 g L−1, accompanied with corresponding γcac and γc0 of 59.29 and 57.85 mN m−1. As the concentration of NaCl is 0.5 g L−1, the values of cac and c0 respectively decrease to 0.38 and 0.76 g L−1. In particular, the corresponding γcac and γc0 obviously drop to 54.37 and 53.62 mN m−1. This reveals that the addition of NaCl reduce the first plateau due to the improvement of surface activity in the mixture. Furthermore, in the γ-logc curves, it is visible that the plateau narrows as the NaCl concentration increases up to 0.5 g L−1. As the concentration of NaCl continues to increase, the plateau eventually disappears, which can be described as “salt weakening effect”. This indicates that the addition of NaCl inhibits the combination of P(NVP-co-MAA) and SLS, producing negative effects on the formation of the mixed system.

Table 6:

Surface chemical property parameters of 0.05 g L−1 P(NVP-co-MAA)/SLS mixed system with different concentrations of NaCl at 25 °C.

Components cNaCl (g L−1) cac (g L−1) γcac (mN m−1) c0 (g L−1) γc0 (mN m−1) cmce (g L−1) γcmce (mN m−1)
0.05 g L−1

P(NVP-co-MAA)

+ SLS		 0 0.40 59.29 0.79 57.85 2.24 42.87
0.5 0.38 54.37 0.76 53.62 2.03 42.68
1 1.58 42.51
2 1.33 41.59

As displayed in Figure S5, the overlaps of the curves from cac to c0 at NaCl concentration of 0.5 g L−1 indicates the presence of the first plateau. Then the plateau disappears with NaCl concentration increasing. This result is in good agreement with that in P(NVP-co-MAA)-SLS system. As seen in Figure 8, the surface tension and cmce decline with the concentration of NaCl increasing. It is implied that the electrostatic interaction between Na+ and SO3 2− of SDS facilitates the SDS molecules to adsorb closer in the interface. As the NaCl concentration reaches to1 g L−1, the “three inflection points corresponding to two plateaus” feature can’t be observed. From Table 7, compared with the mixture without NaCl, the addition of 0.5 g L−1 NaCl makes the values of cac and c0 respectively decrease from 0.61 to 0.49 g L−1 and 0.86 to 0.80 g L−1. It is suggested that in the presence of NaCl (0.5 g L−1), SDS is favorable to interact with P(NVP-co-MAA) at a lower concentration (0.49 g L−1). Meanwhile, the addition of NaCl of 0.5 g L−1 leads to the difference between cac and c0 becoming widen, indicating the extension of the plateau. This result is quite opposite to that in P(NVP-co-MAA)-SLS system even at the same NaCl concentration. In P(NVP-co-MAA)-SDS system, the addition of 0.5 g L−1 NaCl promotes the binding of P(NVP-co-MAA) and SDS, making the mixed system more stable. This situation is considered as “salt enhancement effect” that the addition of NaCl enhances the interaction between P(NVP-co-MAA) and SDS. On the contrary, “salt weakening effect” means the suppression of interaction between P(NVP-co-MAA) and surfactants after adding salt. From the discussion about the two systems above, whether “salt weakening effect” or “salt enhancement effect” is depend on the different surfactants in P(NVP-co-MAA) -containing systems. It is suggested that the surfactants are preferable to interact with the same charged countra-ion. In this study, Na+ has equal charge to COO− rather than SO3 2-, thus the electrostatic attraction between Na+ and COO− group of SLS is stronger. This also results in the binding of SLS and P(NVP-co-MAA) weakening. As shown in Figure 8, in P(NVP-co-MAA) and SDS system, the plateau disappears as the concentration of NaCl exceeds 0.5 g L−1, implying the presence of “salt weakening effect” that hinders the binding of SDS and P(NVP-co-MAA). There exists competition between “salt weakening effect” and “salt enhancement effect”. 40 In P(NVP-co-MAA) and SDS system, “salt enhancement effect” is dominant as the concentration of NaCl within 0.5 g L−1. When the concentration of NaCl continues to increase, the “salt weakening effect” is more important.

Figure 8: The surface tension curves of 0.05 g L−1 P(NVP-co-MAA)/SDS mixed system with different concentrations of NaCl at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).
Figure 8:

The surface tension curves of 0.05 g L−1 P(NVP-co-MAA)/SDS mixed system with different concentrations of NaCl at 25 °C (cac refers to critical aggregation concentration, c0 denotes to saturated binding concentration, cmce represents critical micelle concentration).

Table 7:

Surface chemical property parameters of 0.05 g L−1 P(NVP-co-MAA)/SDS mixed system with different concentrations of NaCl at 25 °C.

Components cNaCl (g L−1) cac (g L−1) γcac (mN m−1) c0 (g L−1) γc0 (mN m−1) cmce (g L−1) γcmce (mN m−1)
0.05 g L−1

P(NVP-co-MAA)

+ SDS		 0 0.61 56.39 0.86 56.03 4.15 28.49
0.5 0.49 50.19 0.80 49.44 4.03 28.31
1 3.98 27.54
2 3.83 26.93

4 Conclusions

In summary, the interactions between P(NVP-co-MAA) and five different surfactants are respectively investigated in this study. The results show that the “three inflection points corresponding to two plateaus” feature appears in the γ-logc curves in P(NVP-co-MAA)-anionic surfactant systems. This indicates that P(NVP-co-MAA) can interact with anionic surfactants (SLS, SDS) mainly by electrostatic attraction. Compared with SLS, SDS exhibits stronger interaction with P(NVP-co-MAA) due to the higher electronegativity (SO3 2−). However, as P(NVP-co-MAA) was added into zwitterionic surfactant solutions (LAB, LHSB), P(NVP-co-MAA) can’t interact with these surfactants. Although LAB and LHSB respectively contain COO− and SO3 2−groups, the presence of quaternary ammonium group on the two surfactants inhibits the binding of P(NVP-co-MAA) and surfactants by electrostatic repulsion. Moreover, P(NVP-co-MAA) can’t bind with cationic surfactant (DTAB) which only has one quaternary ammonium group. This further confirms that the presence of quaternary ammonium group in surfactants inhibits the interaction between polymer and surfactant.

probably because of electrostatic repulsion, steric hindrance and high interaction energy. It follows that P(NVP-co-MAA) is preferable to interact with anionic surfactants instead of zwitterionic and anionic surfactants involving quaternary ammonium group. Finally, NaCl with different concentrations was respectively added into P(NVP-co-MAA)-SLS and P(NVP-co-MAA)-SDS systems. It is found that “salt weakening effect” always exists in P(NVP-co-MAA)-SLS system regardless of NaCl concentration. However, “salt enhancement effect” is dominant in P(NVP-co-MAA)-SDS system at the concentration of NaCl not exceeding 0.5 g L−1. This study sheds light on the interaction between P(NVP-co-MAA) and different surfactants, as well as the corresponding mechanism. In addition, it provides a new guideline for the formulations involving P(NVP-co-MAA) and surfactants applied in household detergents, personal cleaning and care.

Corresponding author: Yuhua Cao, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China, and School of Chemical and Material Engineering, Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, Jiangnan University, Wuxi, 214122, China, E-mail:

About the authors

Yun Zhang

Yun Zhang: PhD candidate in Jiangnan University, major in chemical engineering and technology. His research interests include macromolecular self-assembly, surfactants and daily chemical.

Sihan Yu

Sihan Yu: intermediate engineer, she received master degree from East China University of Science and Technology in 2018, major in Physical Chemistry. She is mainly engaged in the cosmetic research.

Hao Du

Hao Du: postgraduate, he is studying chemical engineering with a focus on amphiphilic polymer, surfactant, bijel and Pickering emulsion.

Yuhua Cao

Yuhua Cao: professor, she received Ph.D. degree from East China Normal University in 2002, major in analytical chemistry. Her reseach interests include amphiphlic random copolymer, surfactants, and photonic crystal.

Hujun Xu

Hujun Xu: professor, he received his Ph.D. degree in 2005 from Nanjing University of Science and Technology, P.R. China. He has been involved in surfactants and detergents for over 30 years. He has published over 70 papers in the field of surfactants and detergents.

  1. Research ethics: Not applicable.

  2. Informed consent: Not applicable.

  3. Author contributions: Yun Zhang: Experimental design, experiment execution, data collection and analysis, figure creation, manuscript writing. Sihan Yu: Experimental design. Hao Du: Experiment execution. Yuhua Cao: Technical support, review and editing. Hujun Xu: Experimental design, technical support, review and editing. All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  4. Use of Large Language Models, AI and Machine Learning Tools: None declared.

  5. Conflict of interest: The authors state no conflict of interest.

  6. Research funding: None declared.

  7. Data availability: Not applicable.

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Supplementary Material

This article contains supplementary material (https://doi.org/10.1515/tsd-2025-2677).

Received: 2025-05-08
Accepted: 2025-09-03
Published Online: 2025-10-21
Published in Print: 2025-11-25

© 2025 Walter de Gruyter GmbH, Berlin/Boston

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  2. Physical Chemistry
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https://doi.org/10.1515/tsd-2025-2677
Keywords for this article
amphiphilic copolymer; surfactant; interaction

Articles in the same Issue

  1. Frontmatter
  2. Physical Chemistry
  3. An anionic micellar approach for the acceleration of catalytic oxidation of L-leucine by KMnO4 in aqueous acidic environment
  4. Sustainability
  5. Lowering the environmental impact of dishwashing and laundry in Europe: a LCA perspective
  6. Synergistic strength enhancement of CDW-based brick using polycarboxylate ether with cement
  7. Application
  8. Investigation on the interactions between amphiphilic copolymer and different surfactants
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