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Surface treatment with plasma, corona, or air and the use of adhesion promoters (primers) are methods that can be used to improve the gluability of various materials. Adhesion promoters based on organosilicone compounds from the solventborne and waterborne catalyzed by isocyanates were used in the study. Dispersions and hot melt adhesives based on various thermoplastic polymers were used. Rheological properties and surface-free energy as well as dispersion and polar shares in substrate-adhesion promoter systems were evaluated. The strength and resistance of glue lines were determined. The tested primers and adhesives were classified as rheostable liquids, diluted in shear, not showing the flow limit. Covering of the surfaces of PVC foils and ABS, PS, PVC edges with primers caused increase in surface-free energy, especially polar share. Significant improvement of strength and resistance of glue-lines was observed (100% delamination in the substrate).
Laboratory of Gluing and Finishing of Surface, Department of Wood Science and Thermal Techniques, Poznan University of Life Sciences, Poznan, Poland
*Address all correspondence to: tomasz.krystofiak@up.poznan.pl
1. Introduction
In the last 20 years, the production of different furniture has increased. With the continuous development of the furniture industry, research work on the various products and surfaces used in furniture is important and justified. They support the industry in its continuous development and aspiration of ever better quality and sales results.
In various areas of the furniture industry and interior design, various types of materials are increasingly being introduced, often representing surfaces with limited susceptibility to gluing. These include primarily plastics in edge tapes based on ABS (acrylonitrile butadiene styrene), PA (polyamide), PE (polyethylene), PMMA (polymethyl methacrylate), and PVC (polyvinyl chloride) [1].
They are used for wrapping narrow surfaces of panel elements in standard technology, soft forming, and machining centers [2, 3]. In particular, the problems with wrapping are caused by the edges used for office furniture, kitchen furniture, and interior design. They exhibit high rigidity and the resulting limited susceptibility to deformation, which is due to their relatively significant thickness reaching values up to 5 mm [4, 5, 6, 7, 8, 9]. Materials with hard-to-glue surfaces include laminates produced in HPL (high-pressure laminate) or LPL (low-pressure laminate) versions, for example, are intended for postforming finishing of the surface of panel elements. The theoretical basis for possible adhesive interactions in adhesive-substrate systems in relation to plastics has been presented in numerous studies [10, 11, 12]. These publications do not take into account the specific surface properties of these materials, which can significantly affect the course of gluing processes, adhesion phenomena, and thus the strength and resistance of glue lines [13].
It is generally accepted that difficulties in gluing various polymeric materials are caused by their nonporous surface and relatively low surface-free energy, usually at the level of 30–40 mJ/m2. The surfaces of many plastics have a nonpolar character, which is also considered one of the main reasons for limited gluability, especially since adhesives usually have a polar character. In these cases, the aim is to give polarity to nonpolar surfaces immediately before gluing through their special preparation. Duroplast-based plastics are characterized by a smooth, compact, low-porous surface, and high resistance to solvents, which practically eliminates the processes of penetration. In the case of these materials, serious difficulties can be observed during the curing of adhesives, associated with the evaporation of volatile components, which in turn may cause porosity of glue lines and reduce the quality of joints [14].
A significant influence on the bonding of plastics can be executed by a specific technique of their production, for example, extrusion, rolling, pressing, casting, extrusion, calendering, and vacuum forming. Individual processing methods affect both the macroscopic structure and the location of chemical groups on the surface of the material. It should also be noted that in many operations in the field of plastics production, various adhesion promoters are used to cover the surface of individual industrial equipment in given technologies to facilitate processes. The reason for inadequate gluing may be the content in plastics of various types of agents from the auxiliary group, for example, plasticizers. Plasticizers during the processing process may migrate to the glued surface and adversely affect the bonding processes, for example, by inhibiting the hardening processes of the adhesive [15].
Adhesives are then used in a properly selected set of solvents, which cause the effect of short-term plasticization of the surface of the varnish coatings [16].
From the practical point of view, an important criterion flowing from the adsorption theory of adhesion and allowing to determine the suitability of an adhesive for joining a given material is the appropriate contact angle and the surface tension of the adhesive and the surface-free energy of the surface to be glued [17]. According to literature data, the surface-free energy (γS) of the glued material should be higher by at least 10 mJ/m2 than the γS of the used adhesives. This is required due to the need for proper wetting of the surface by adhesives and thus meeting the thermodynamic adhesion condition [18]. In order to increase the γS of plastics to the values appropriate for a given adhesive, their top layer can be modified, for example, by removing migrating auxiliary components from the surface and developing the geometric structure [19].
In particular, an interesting area of research turned out to be the issue of wettability, surface-free energy of glued materials and the search in the light of the assumptions of adsorption theory of adhesion, interdependence in the scope of specified characteristics and the strength of the obtained glue lines [20, 21].
The aim of this study was to determine the rheological properties of adhesion promoters, wettability properties, and the strength and thermoresistance of the obtained joints.
To carry out the experiments, adhesion promoters based on OSI were used in the version of one-component solvent products (from the aminosilane group) and in the form of two-component waterborne products (from the group catalyzed with isocyanates). In Table 1 properties of solvent-borne and in Table 2 waterborne adhesion promoters are given.
Property
Marking
S-1
S-2
S-3
S-4
S-5
S-6
Color
Transparent
Yellow
White
Green
Green
Transparent
Density [g/cm3]
0.90
0.90
0.85
0.90
0.90
0.90
Dynamic viscosity [mPa.s]
140
300
35
50
60
30
Solid content [%]
14
16
13
12
12
12
Recommended amount of application [g/m2]
5–10
Destination
Foils and edges
Table 1.
Properties of the solvent-borne adhesion promoters [13].
Property
Marking
W-1
W-2
W-3
W-4
Color
Green
Yellow
Yellow
Transparent
Density [g/cm3]
1.0 ± 0.05
Dynamic viscosity [mPa.s]
1000
1000
30 ± 10
600 ± 200
Solid content
27
28
30 ± 2
25 ± 2
pH value
7.5 ± 0.5
Recommended amount of application [g/m2]
5–10
Destination
Foils and edges
Table 2.
Properties of the waterborne adhesion promoters [13].
In the initial experimental phase, a total of 10 commercial products offered by Jowat AG in Detmold/Germany/were tested, including six solvents and four waterborne ones. Selected properties of these adhesion promoters on the basis of own tests and information obtained from the manufacturer are given respectively in Tables 1–2.
Taking into account the results of preliminary experiments, two adhesion promoters marked in the work as S-1 (solventborne) and W-1 (waterborne) were selected for the investigations.
2.2 Adhesives
For profile wrapping of edges of panel elements, HM (hot melt) adhesives based on EVA (ethylene vinyl acetate) in the version with or without fillers, APAO (alpha-polyolefins), PA (polyamide), and PUR (polyurethane) are mainly used. They are characterized by many advantages in the ability to wet substrates with different polarity, good pre-adhesion, short open time, high setting speed, high resistance of glue lines to tearing, and beneficial features from the point of view of environmental protection, which predestines them for numerous applications in woodworking industry [22, 23].
Taking into account the consolidating trends, especially in kitchen and office furniture, manufacturers are increasingly introducing multicolored, with different thickness of edges, for example, based on ABS, PVC, PS polymers. Adhesives used to glue these edges are required, first of all, with very good adhesion and obtaining a transparent and thin adhesive glue line. In this context, it is increasingly common to use HM EVA adhesives without filler and reactive PUR, ensuring obtaining glue lines with increased strength and thermal resistance [24, 25, 26].
2.3 Edges
The current range of offered types and varieties of foil and edging is very diverse, meeting the numerous expectations and requirements of designers, manufacturers, and users of individual final products.
Edges based on ABS, PS, and PVC were selected, also in the version without the adhesion promoters from the offer of products made in the technical conditions of PPUH SILPLAST/Poland Company/. Edges with a thickness of 3.0 mm and a width of 22 mm in the form of coils with a length of 100 m were purchased directly from their manufacturer. The properties of edges, based on the manufacturer’s data, are presented in Table 3.
Property
Polymer basis
ABS
PS
PVC
Hardness acc. to DIN 53505 standard (Shore methods) [N/mm2]
73
75
81
Coefficient of thermal expandability [1/K × 10−6]
85
95
80
Shrinkage (1 h in 90°C) [%]
< 0.3
< 0.7
< 2.0
Thermoresistance acc. to DIN 53460 standard (Vicat resistance) [°C]
96
90
78
Resistance to UV radiation acc. to the DIN 53388 standard
6.0
6.0
6.0–7.0
Resistance to cold liquid action acc. to the DIN 68861 standard (grade scale)
ABS, PS, and PVC edge tapes were selected for the research. The primers were applied in the laboratory (at 20 ± 2 °C and RH = 65 ± 5%). With the help of metal spreading strips (rakels), solvent-based and waterborne adhesion promoters were applied in the amount of 15 and 8 g/m2, respectively. The solidification process was carried out under the following conditions:
edging with temp. 20 ± 2°C, solidification under RT conditions
edging with temp. 20 ± 2°C, forced air dryer solidification (60, 80 and 100°C, time 3 and 5 min)
edging with temp. 60 ± 2°C, solidification in a forced air dryer (temp. 60, 80 and 100°C, time 3 min).
2.5 Preparation of samples for strength estimation and thermal resistance of glue lines
The process of edgebanding of particleboards with dimensions of 200 x 200 x 19 mm with ABS, PS, and PVC edges with applied primers was made using HM adhesives in the edgebanding prototype machine.
The tear strength tests were carried out in the Zwick 1445 test machine equipped with standard tooling in a set of rollers enabling tearing at an angle of 90°, at a loading speed of 1000 mm/min.
Visually, the degree of delamination occurring in the glued substrate under destructive loadings was carried out using the adopted scale (Table 4).
Grades
Delamination degree [%]
1
100
2
≥90
3
≥80
4
≥60
5
<60
Table 4.
Adopted scale for the assessment of the results of the tests of the resistance of glue lines to tearing [13].
The determination of the thermal resistance of the glue lines contained in the narrow surfaces of the panel elements was made with a gradual increase in temperature. The samples were placed in a laboratory dryer with forced air circulation heated to 50 ± 2°C and heated. After 1 hour, the samples were subjected to a detailed visual assessment of the glued surfaces, checking whether they had not delaminated. If no delamination was found, the samples were placed in a dryer at a temperature of 60 ± 2°C and after 1 hour of soaking, another visual inspection was carried out. The determination was carried out until the first signs of deformation of the glue lines. If no delamination occurred, the tests were discontinued at 150°C.
2.6 Investigations of the rheological properties
The tests were carried out with the Rheotest-2 rotational rheoviscometer, conducting measurements at shear rates in the range of 2.7–1312 s−1 as a function of temperature 15, 20, 25, and 30°C. Based on the experience of rheometric data, shearing stresses and apparent viscosity were determined.
Subsequently, the experimental data were approximated to the appropriate rheological model and the values of its parameters were determined. Based on earlier research results, a rheological power model of Ostwald de Waele was used in the form of:
τ=k.γn1E1
in which:
τ—shear stresses
k—coefficient of consistence
γ—shear rate [s−1]
n1—exponent
In turn, the analysis of rheological models describing the relationship ή, = f (τ) for rheostable fluids allowed to conclude that in the studied area of γ experimental data can be correctly approximated using the three-parameter Ellis model, in the form of:
η,=η0/1+η/η1/2α1−1E2
The parameters of this model are
η0 (Pa. s)—viscosity in the Ellis model
τ1/2 (Pa)—shear stresses in the Ellis model
α1—rheological parameter
For the approximation of experimental data to the formula of the Ellis model, the random Brooks gradient method was used [13].
2.7 Wettability
The surface of the substrate subjected to gluing should be characterized by adequate wettability. Appropriate adhesion between the substrate (foil, edge) and the binder (primer, glue) is possible only if monolayers and molecular contact are formed between the wetting liquid and the material [13, 27].
On the basis of the assumptions of adsorbent adhesion theory and the Young-Dupre equation, it is possible to determine adhesive relations based on the value of the interactions of surface forces of contacting materials [28, 29, 30].
One of the most important adhesive parameters is surface-free energy together with dispersion and polar shares [31, 32].
It was assumed that good bonding is achieved when the surface-free energy of the substrate was higher than the surface tension of the wetting liquid.
Measurements of the angle of wetting with redistilled water were carried out with a PG-3 pocket goniometer, recording the results 15 s after applying a drop of redistilled water.
On the basis of the obtained results, surface-free energy was determined together with dispersion and polar shares [31, 33].
Table 5 shows the values of the rheological parameters of this model and the correlation coefficients. The values of r2 obtained in the calculations indicate the accuracy of the selection of the approximated rheological model. For all the cases under consideration, the power exponent n1 < 1, which, according to literature data, confirms that these systems decreases with increasing γ. The systems in question therefore represent the category of rheostable liquids, not showing a flow limit, diluted by shear. In Polish literature, these fluids are referred to as pseudoplastic, while in foreign-language literature, they are called liquids with apparent viscosity.
Amount of hardener [%]
Temperature [°C]
Model parameters
Correlation coefficient R2
k [Pa.s]
n1 [−]
[−]
0
15
6.83
0.67
0.987
20
6.08
0.67
0.987
25
6.30
0.66
0.978
30
3.74
0.73
0.985
2.5
15
7.87
0.65
0.988
20
8.33
0.63
0.987
25
6.96
0.65
0.992
30
6.45
0.65
0.986
5.0
15
7.91
0.62
0.991
20
6.80
0.66
0.982
25
5.14
0.68
0.990
30
2.54
0.77
0.994
Table 5.
Influence of the amount of catalyst added to the waterborne adhesion promoter on the formation of rheological parameters of the Ostwald de Waele model as a function of temperature [13].
Analysis of the data in Table 5 shows that the most sensitive rheological parameter in the Ostwald de Waele model, subject to noticeable changes in the range of factors under consideration, is the consistency coefficient k1, whose values are in the range of 2.54–8.33. A general analysis of the obtained data indicates that as the share of the catalyst in the system increases, there is a tendency to increase the value of the k1 factor. It can also be stated that a clear decrease in the value of this coefficient occurs with an increase in temperature. In turn, the power exponent n1, which is a measure of the deviation of a given fluid from the Newtonian liquid, undergoes much smaller fluctuations at the level of 0.6–0.7. The more the values of n1 differed from unity, the more pronounced the non-Newtonian properties of a given liquid became.
The values of the rheological parameters determined for each system in the Ellis model are given in Table 6. By assessing the course of changes in the values of rheological parameters in the Ellis model determined for individual systems, it is possible to determine certain regularities in the parameters of limit viscosity η0 and shearing stress τ1/2 at different measurement temperatures. The values of parameter a were in the numerical range of 0.69–1.02 decreasing with increasing temperature and the share of the hardener in the W-1 adhesion promoter. According to [34], relations in terms of the formation of values η0 and τ1/2 for the studied systems can be expressed by means of an indicator constituting the quotient of the value of these parameters, called the characteristic fluid time. Table 6 summarizes the calculated values of this indicator.
Amount of hardener
Temperature
Model parameters
Characteristic time
[%]
[°C]
ηo [Pa.s]
τ½ [Pa]
α1 [−]
ηo/τ½ [−]
0
15
0.17
0.21
1.02
0.81
20
0.14
0.20
0.87
0.70
25
0.12
0.20
0.83
0.60
30
0.10
0.19
0.77
0.53
2.5
15
0.15
0.22
0.91
0.68
20
0.14
0.21
0.87
0.67
25
0.12
0.20
0.83
0.60
30
0.11
0.20
0.80
0.55
5.0
15
0.14
0.22
0.87
0.64
20
0.12
0.20
0.84
0.60
25
0.10
0.19
0.77
0.53
30
0.08
0.17
0.69
0.47
Table 6.
Influence of the amount of catalyst added to the waterborne adhesion promoter on the formation of rheological parameters in the Ellis model as a function of measurement temperature.
Analysis of the data contained in this table proves that the participation of the catalyst in the W-1 adhesion promoter causes an increase in the value of the parameter α1.
3.2 Wettability
When presenting the results in the field of wettability, the citation and detailed analysis of the wetting angle values obtained in the measurements, which were used to carry out the relevant calculations, were abandoned, focusing mainly on discussing the relationship in the formation of surface-free energy for individual substrate-adhesion promoter-adhesive systems.
For substrates covered with adhesion promoters included in the work, the values of surface-free energy (γS) were determined on the basis of measurements of the angle of wetting with redistilled water, together with the dispersion (γSd) and polar (γSp) shares.
Figure 1 presents the relevant values for the surface-free energy with dispersion and polar shares for tested surface with and without adhesion promoters. A general analysis of these data indicates that both film and periphery tapes are characterized by very low values of γS contained depending on the base polymer in the range of 28.42–39.17 mJ/m2. Covering the surface of these materials with adhesion promoters resulted in a clear increase in the value of γS, extremely beneficial from the point of view of the theoretical assumptions of adsorption theory of adhesion. These changes occurred primarily due to an increase in the polar component. For example, for PS-based edge tape, the value of this component after covering the surface with individual adhesives changed from 1.26 to over 13 mJ/m2. In the comparative system, a slightly more effective solution for this group of substrates turned out to be a waterborne adhesion promoter in a catalyzed version.
Figure 1.
Surface-free energy (γS) including dispersion (γSd) and polar (γSp) shares for edges covered with adhesion promoters.
3.3 Peel strength
A clear influence of the type of adhesive on the strength of glue lines in the edgebanded boards was also observed. In Figure 2 results of the strength estimation are given.
Figure 2.
Influence of adhesion promoter into peel strength.
A general analysis of the presented data proves that the type of adhesive significantly affects the quality of the joints. The non-stick coating of the surface of the edge tapes resulted in a clear improvement in the share of damage in the substrate during the delamination of the glue lines, respectively, from HM PUR glue from 80–85% (grade 3) to 100% (grade 1), in the case of HM APAO from 65% (grade 4) to 100% (grade 1), HM EVA without filler from 50% (grade 5) to 85–95% (grade 1–2 depending on the type of edging tape), and what should be emphasized for HM with filler from 20% (grade 5) up to 80% (Grade 3). Therefore, the tested HM adhesives can be ranked in terms of tear strength as follows (from the highest to the lowest):
PUR≥APAO>EVAwithoutfiller>EVAwithfiller
It can be concluded that the glue lines obtained as a result of the use of adhesion promoters for the preparation of the surface of foil and edging tapes for gluing constitute in terms of tearing strength, carried out, which should be exposed in conditions of shock forces at a load rise rate of 1000 mm / min, a coherent, high-quality system, the weakest link of which is the chipboard substrate, delamination at relatively low values of destructive loadings.
3.4 Thermoresistance of glue lines
In Figure 3, results of the thermoresistance are given. A very significant effect of the type of glue on the thermal resistance of glue lines was found. The use of adhesion promoters resulted in an increase in the thermal resistance of joints for individual edge tapes and HM adhesives respectively for: EVA without filler 43–57% (30–40°C), APAO by 44–63% (+40–50°C), PUR by 36–50% (+40–50°C), EVA with filler 33–40% (+20°C). In terms of thermal resistance of glue lines from narrow surfaces of plate elements with edges HM adhesives (from the highest to the lowest) can therefore be ranked as follows:
Figure 3.
Influence of adhesion promoter into thermoresistance of glue lines from HM adhesives.
PUR>APAO>EVAwithoutfiller>EVAwithfiller
however, taking into account the relative increase in thermal resistance:
APAO>EVAwithoutfiller>PUR>EVAwithfiller
Analyzing the type of edge material used for edgebanding, it can be concluded that the most advantageous product in terms of heat resistance in comparison with particleboard and adhesives included in the experiments is PVC edge, while ABS and PS turned out to be slightly inferior (the level of heat resistance lower by 10–20°C). It certainly results from the formation of mechanical and thermal properties of the base polymers of the tapes during heating. In the course of conducting, these studies, for example, changes in the thermal expansion of the tested tapes were observed during the experiments. In the case of ABS and PS edges, the maximum thermal expansion over the sample length of 2 mm was recorded at the time of delamination of the glue lines.
In the application works carried out in laboratory and industrial conditions, it was established that the solvent-borne adhesion promoter should be applied to individual substrates in the form of thin layers in the amount of at least 15 g/m2 and solidified at an air temperature of 20 ± 2°C and RH = 65 ± 5% in about 5 minutes. On the other hand, a waterborne adhesion promoter with the participation of a 5% isocyanate catalyst in an amount of at least 8 g / m2 and after drying at 60°C for 5 min.
Carried out research has indicated the opportunity of using solvent-borne and waterborne adhesion promoters for furniture production.
The waterborne adhesion promoters were classified as rheostable liquids diluted by shearing not showing a flow limit (pseudoplastic liquids). There was no effect of the hardener on the rheological characteristics of the adhesion promoter mixtures.
The greatest usefulness for approximating experimental data in terms of descriptions of flow curves was shown by the of Ostwald de Waele rheological model. The most sensitive parameter in this model was the consistency factor k1. Along with the increase in the share of the catalyst, the value of this coefficient increased.
The Ellis model showed the greatest usefulness for the approximation of experimental data describing the relationship of the formation of apparent viscosity in the function of shearing stresses. The values of the rheological parameter characteristic in this model α1 decreased with the increase in the temperature of the system and the amount of catalyst.
Covering the ABS, PS, PVC edge surfaces with adhesion promoters caused a clear increase in surface-free energy. These changes occurred primarily due to an increase in the polar share.
Adhesion promoters on the ABS, PS, PVC edge surfaces caused a clear improvement in the delaminations of glue lines in the substrate.
The use of adhesives resulted in an increase in the thermal resistance of joints from edges and HM adhesives.
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Written By
Tomasz Krystofiak
Submitted: 13 June 2022Reviewed: 06 July 2022Published: 17 August 2022
Open access peer-reviewed chapter
