Citation: Lubis, M.A.R.; Labib, A.;
Sudarmanto; Akbar, F.; Nuryawan,
A.; Antov, P.; Kristak, L.;
Papadopoulos, A.N.; Pizzi, A.
Influence of Lignin Content and
Pressing Time on Plywood Properties
Bonded with Cold-Setting Adhesive
Based on Poly (Vinyl Alcohol),
Lignin, and Hexamine. Polymers 2022,
14, 2111. https://doi.org/10.3390/
polym14102111
Academic Editors: Francesco Paolo
La Mantia and Charles Frihart
Received: 4 April 2022
Accepted: 20 May 2022
Published: 22 May 2022
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polymers
Article
Influence of Lignin Content and Pressing Time on Plywood
Properties Bonded with Cold-Setting Adhesive Based on Poly
(Vinyl Alcohol), Lignin, and Hexamine
Muhammad Adly Rahandi Lubis
1,2,
* , Ahmad Labib
3
, Sudarmanto
1
, Fazhar Akbar
1
, Arif Nuryawan
3,
* ,
Petar Antov
4
, Lubos Kristak
5
, Antonios Nikolaos Papadopoulos
6,
* and Antonio Pizzi
7
1
Research Center for Biomass and Bioproducts, National Research and Innovation Agency of Indonesia,
Cibinong 16911, Indonesia; sudarmantokm46@gmail.com (S.); fazharbio46@yahoo.co.id (F.A.)
2
Research Collaboration Center for Biomass and Biorefinery between BRIN and Universitas Padjadjaran,
National Research and Innovation Agency of Indonesia, Cibinong 16911, Indonesia
3
Department of Forest Products Technology, Faculty of Forestry, Universitas Sumatera Utara,
Kwala Bekala Campus, Medan 20355, Indonesia; alabib602@gmail.com
4
Faculty of Forest Industry, University of Forestry, 1797 Sofia, Bulgaria;p.antov@ltu.bg
5
Faculty of Wood Sciences and Technology, Technical University inZvolen, 96001 Zvolen, Slovakia;
kristak@tuzvo.sk
6
Laboratory of Wood Chemistry and Technology, Department of Forestry and Natural Environment,
International Hellenic University, GR-661 00 Drama, Greece
7
LERMAB, Faculte des Sciences, University of Lorraine, Blvd. des Aiguillettes, 54000 Nancy, France;
antonio.pizzi@univ-lorraine.fr
* Correspondence: marl@biomaterial.lipi.go.id (M.A.R.L.); arif5@usu.ac.id (A.N.); antpap@for.ihu.gr (A.N.P.)
Abstract: The sustainability, performance, and cost of production in the plywood industry depend
on wood adhesives and the hot-pressing process. In this study, a cold-setting plywood adhesive
was developed based on polyvinyl alcohol (PVOH), high-purity lignin, and hexamine. The in-
fluence of lignin content (10%, 15%, and 20%) and cold-pressing time (3, 6, 12, and 24 h) on co-
hesion, adhesion, and formaldehyde emission of plywood were investigated through physical,
chemical, thermal, and mechanical analyses. The increased lignin addition level lowered the solids
content, which resulted in reduced average viscosity of the adhesive. As a result, the cohesion
strength of the adhesive formulation with 10% lignin addition was greater than those of 15% and
20% lignin content. Markedly, the adhesive formulation containing a 15% lignin addition level
exhibited superior thermo-mechanical properties than the blends with 10% and 20% lignin content.
This study showed that 10% and 15% lignin content in the adhesive resulted in better cohesion
strength than that with 20% lignin content. However, statistical analysis revealed that the addition
of 20% lignin in the adhesive and using a cold-pressing time of 24 h could produce plywood that
was comparable to the control polyurethane resins, i.e., dry tensile shear strength (TSS) value of
0.95 MPa, modulus of rupture (MOR) ranging from 35.8 MPa, modulus of elasticity (MOE) values
varying from 3980 MPa, and close-to-zero formaldehyde emission (FE) of 0.1 mg/L, which meets
the strictest emission standards. This study demonstrated the feasibility of fabricating eco-friendly
plywood bonded with PVOH–lignin–hexamine-based adhesive using cold pressing as an alternative
to conventional plywood.
Keywords: adhesion; bio-based adhesives; cold pressing; cohesion; formaldehyde emission; hexamine;
lignin; PVOH; wood-based panels; plywood
1. Introduction
The sustainability, performance, and cost of production in the plywood industry
depend on wood adhesives and the hot-pressing process [1,2]. Plywood is produced
dominantly using urea-formaldehyde (UF) resins, with an estimated global consumption
Polymers 2022, 14, 2111. https://doi.org/10.3390/polym14102111 https://www.mdpi.com/journal/polymers