• Journal of the Korean Wood Science and Technology
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• v.49 no.2
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• pp.169-180
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• 2021

Inherent crystalline domains present in low formaldehyde to urea (F/U) molar ratio urea-formaldehyde (UF) resins are responsible for their poor adhesion in wood-based composite panels. To modify the crystallinity of low molar ratio (LMR) UF resins, this study investigates the additional effect of cellulose nanomaterials (CNMs), such as cellulose microfibrils (CMFs), cellulose nanofibrils (CNFs), and TEMPO-oxidized CNFs (TEMPO-CNFs) on the crystallinity of modified LMR UF resins. First, two modification methods (post-mixing and in situ) were compared for modified LMR UF resins with TEMPO-CNFs. The modified UF resins with TEMPO-CNFs decreased the nonvolatile solid contents, while increasing the viscosity and gel time. However, the in situ modification of UF resins with TEMPO-CNFs showed lower crystallinity than that of post-mixing. Then, the in situ method was compared for all CNMs to modify LMR UF resins. The modified UF resins with CMFs using the in situ method increased nonvolatile solid contents and viscosity but decreased the gel time. The crystallinity of UF resins modified with TEMPO-CNFs was the lowest even though the crystalline domains were not significantly changed for all modified UF resins. These results suggest that these CNMs should be modified to prevent the formation of crystalline domains in LMR UF resins.

• Journal of the Korean Wood Science and Technology
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• v.47 no.2
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• pp.221-228
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• 2019

This study reports the performance of urea-formaldehyde (UF) resins prepared at two different low formaldehyde/urea (F/U) mole ratios with different numbers of urea addition during synthesis. The second or third urea was added during the synthesis of UF resins to obtain two different low molar ratios of 0.7 and 1.0, respectively. The molecular weights, cure kinetics, and adhesion performance of these resins were characterized by the gel permeation chromatography, differential scanning calorimetry, and tensile shear strength of plywood, respectively. When the number of urea additions and F/U molar ratio increased, the gelation time decreased, whereas the viscosity and molecular weight increased. Further, the UF resins prepared with the second urea and 1.0 molar ratio resulted in greater activation energy than those with third urea and 0.7 molar ratio. Tensile shear strength and formaldehyde emission (FE) of the plywood that bonded with these resins increased when the number of urea additions and molar ratio increased. These results suggest that the UF resins prepared with 0.7 molar ratio and third urea addition provide lower adhesion performance and FE than those resins with 1.0 mole ratio and the second urea addition.

• Journal of the Korean Wood Science and Technology
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• v.48 no.2
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• pp.136-153
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• 2020

In this paper, the influence of initial formaldehyde/urea (F/U) molar ratios on the performance of low molar ratio (1.0) urea-formaldehyde (UF) resin adhesives has been investigated. Two initial F/U molar ratios, i.e., the first and second initial molar ratios were used for the alkaline addition reaction. Three levels of the first initial F/U molar ratios (2.0, 3.0, and 4.0) and two levels of the second initial molar ratios (2.0 and 1.7) were employed to prepare a total of six UF resins with an identical final molar ratio (1.0). The basis properties, functional groups, molecular weight, crystallinity, and thermal curing properties of the UF resins were characterized in detail. Higher levels (3.0 and 4.0) of the first initial F/U molar ratio provided the UF resins with better properties (non-volatile solids content, viscosity, gelation time, pH, and specific gravity) than those of the resins prepared with the conventional level F/U molar ratio of 2.0. Statistical analysis suggested that combining the first and second initial molar ratio of 4.0 with 1.7 would result in UF resins with greater adhesion strength and lower formaldehyde emission than those of the resins prepared with other molar ratios. The results showed that higher levels of the first initial molar ratio resulted in a more branched structure, as indicated by GPC, FTIR, DSC, XRD, and greater adhesion strength than those of the other UF resins with an identical final molar ratio of 1.0.

• Journal of the Korean Wood Science and Technology
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• v.49 no.5
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• pp.453-461
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• 2021

In wood-based composite panels, low-molar ratio (LMR) urea-formaldehyde (UF) resins usually result in reduced formaldehyde emission (FE) at the expense of poor adhesion. However, the FE and adhesion of medium-density fiberboard (MDF) bonded with LMR UF resins were both improved in this study. The modified LMR UF resins with transition metal ion-modified bentonite (TMI-BNT) nanoclay simultaneously improved the FE and adhesion of MDF panels. The modified LMR UF resins with 5% TMI-BNT resulted in a 37.1% FE reduction and 102.6% increase in the internal bonding (IB) strength of MDF panels. Furthermore, thickness swelling and water absorption also significantly decreased to 13.0% and 24.9%, respectively. These results imply that TMI-BNT modification of LMR UF resins could enhance the formation of a three-dimensional network rather than crystalline domains, resulting in improved cohesion.

• Journal of the Korean Wood Science and Technology
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• v.50 no.5
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• pp.353-364
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• 2022

The crystalline domain of thermosetting urea-formaldehyde (UF) resins at low formaldehyde-to-urea (F/U) molar ratios (≤ 1.0) is known to be responsible for their poor performance as wood adhesives. Crystallization has been observed in 1.0 F/U UF resins during the addition reaction stage and at the end of the synthesis process (neat UF resins). The crystallinity and X-ray diffraction (XRD) spectra of the uncured neat UF resins, on the other hand, differed significantly from those of the cured neat UF resins, raising the possibility that their crystal structures were also different. This study demonstrates for the first time that the crystalline domains in 1.0 F/U UF resins generated from uncured and cured samples are identical. Despite having a lower crystallinity value, the synchrotron XRD patterns of purified neat UF resins were equivalent to the XRD patterns of cured neat UF resins. Transmission electron microscope images of the cured UF resins showed that the crystals were lamellar structures. This finding suggests that the crystal at low molar ratio UF resins are isotropic polycrystals with random orientation.