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Special Issue "Renewable Polymeric Adhesives II"

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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Circular and Green Polymer Science".

Deadline for manuscript submissions: closed (31 March 2022) | Viewed by 11297

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Prof. Dr. Antonio Pizzi

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LERMAB, Laboratoire d’Etude et de Recherche sur le MAteriau Bois, Université de Lorraine, 27 rue Philippe Seguin, CS60036, 88021 Epinal, France
Interests: polycondensation; resins; adhesives; thermosetting polymers for adhesives; natural polymers for industrial use; fibrous and wood composites; polymeric wood constituents (cellulose, lignin, tannins)
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Special Issue Information

Dear Colleagues,

We are welcoming submissions to the second issue of “Renewable Polymeric Adhesives”. Due to the great interest in the first issue and the considerable number of citations of the ensemble of papers that were published within, the Editorial Board decided to reopen this Special Issue to focus on technologies currently emerging in the field of adhesives and binders.

Renewable polymeric adhesives is an area for which interest is growing for all areas of polymer chemistry and polymer applications, and an area of primary development area for “green” chemistry. Adhesives in this area are inevitably coming of age, and coming rather rapidly. Thus, proteins such as soy proteins, albumin, and gluten; as well as their combinations with carbohydrates such as in soy flour; natural polyphenolics such as a variety of tannins and lignins; carbohydrates such as chitosans, glucose, sucrose, sorbitol, and others; as well as all sorts of sustainable, renewable materials such as citric acid, isorsobide, cashewnut liquid, and others are starting to find their place as total binders or even as partial support for synthetic polymers in many areas of adhesion: from wood and natural fibres to steel, aluminium, and other metals, plastics, glass fibres, foundry sands, and many others.

This Special Issue is aimed at collecting cutting-edge original research papers and reviews on the main areas where biosourced polymeric adhesives from renewable materials are under development and under particular focus, and throughout the vast variety of adhesives in use today, from acrylics to epoxies, polyurethanes, and all others.

Prof. Dr. Antonio Pizzi
Guest Editor

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

biosourced polyurethane adhesives
biosourced acrylic adhesives
biosourced epoxy adhesives
biosourced phenolic adhesives
biosourced aminoplastic adhesives
biosourced furanic adhesives
protein adhesives

Published Papers (6 papers)

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Research

Open AccessArticle

Highly Branched Tannin-Tris(2-aminoethyl)amine-Urea Wood Adhesives

and

Polymers 2023, 15(4), 890; https://doi.org/10.3390/polym15040890 - 10 Feb 2023

Cited by 5 | Viewed by 1120

Abstract

Condensed tannin copolymerized with hyperbranched tris(2-aminoethyl)amine-urea formed by amine-amido deamination yields a particleboard thermosetting adhesive without any aldehydes satisfying the requirements of relevant standards for the particleboard internal bond strength. The tannin–triamine–urea cures well at 180 °C, a relatively low temperature for today’s particleboard hot pressing. As aldehydes were not used, the formaldehyde emission was found to be zero, not even in traces due to the heating of wood. The effect is ascribed to the presence of many reactive sites, such as amide, amino, and phenolic groups belonging to the three reagents used. The tannin appears to function as an additional cross-linking agent, almost a nucleating agent, for the triamine–urea hyperbranched oligomers. Chemical analysis by MALDI ToF and ¹³C NMR has shown that the predominant cross-linking reaction is that of the substitution of the tannin phenolic hydroxyls by the amino groups of the triamine. The reaction of tannin with the still-free amide groups of urea is rather rare, but it may occur with the rarer tannin flavonoid units in which the heterocyclic ring is opened. Due to the temperature gradient between the surfaces and the board core in the particleboard during hot pressing, the type and the relative balance of covalent and ionic bonds in the resin structure may differ in the surfaces and the board core. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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Open AccessArticle

A Green Resin Wood Adhesive from Synthetic Polyamide Crosslinking with Glyoxal

and

Guanben Du

Polymers 2022, 14(14), 2819; https://doi.org/10.3390/polym14142819 - 11 Jul 2022

Cited by 2 | Viewed by 1473

Abstract

Glyoxal is considered to be the most likely substitute for formaldehyde to synthesize resin adhesives for wood bonding due to its reactivity, structural characteristics, being non-toxic, low volatility, and acceptable cost. Regrettably, the performance of the resin synthesized using glyoxal to directly replace all formaldehyde is not totally satisfactory, especially as it has almost no water resistance. This makes such a simple alternative fail to be suitable for industrial production. To prepare an environment-friendly glyoxal-based adhesive with good bonding performance, the work presented here relies first on reacting citric acid and hexamethylene diamine, producing a polyamide, with glyoxal, and then crosslinking it, thus synthesizing a thermosetting resin (namely CHG) adhesive and applying it for plywood bonding. The plywood prepared exhibits excellent dry and wet shear strength, which are better than GB/T9846-2015 standard requirements (≥0.7 MPa), and even after being soaked in hot water at 63 °C for 3 h, its strength is still as high as 1.35 MPa. The CHG resin is then potentially an adhesive for industrial application for replacing UF (urea-formaldehyde) and MUF (melamine-urea-formaldehyde) adhesives for wood composites. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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Open AccessArticle

Improved Wood-Bond Strengths Using Soy and Canola Flours with pMDI and PAE

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Polymers 2022, 14(7), 1272; https://doi.org/10.3390/polym14071272 - 22 Mar 2022

Cited by 3 | Viewed by 1185

Abstract

The surprising lack of literature on using the very common wood adhesive polymeric methylenediphenyl diisocyanate (pMDI) with protein adhesives may be because of perceived poor improvement of protein wet strength. Reacting pMDI with the flour (soy or canola) before adding water unexpectedly improves wood bonding compared to adding the pMDI to an aqueous protein slurry. Mixing the liquid pMDI with the oilseed flour produces a free-flowing powder with up to 50% of pMDI to flour by weight. The mixture slowly reacts since the isocyanate band in the infrared spectra remains for several days but diminishes with time. Adding pMDI increases the dry and wet strength of wood bonds using Automated Bonding Evaluation System (ABES) testing and levels off at about 50%. Similarly, adding the polyamidoamine-epichlorohydrin (PAE) cross-linker to the oilseed flour increases dry and wet bond strength, but the effect levels off at about 20% of PAE. However, the combination of these two cross-linkers added to the flours results in greater dry and wet shear strength than either one alone. In addition to tests using ABES (ASTM D 7998), the increase in strengths is also observed—but with a diminished effect—in bonding plywood using the interior plywood strength test ASTM D 906. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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Open AccessArticle

A Study of Concept to Prepare Totally Biosourced Wood Adhesives from Only Soy Protein and Tannin

Saman Ghahri

Antonio Pizzi

and

Reza Hajihassani

Polymers 2022, 14(6), 1150; https://doi.org/10.3390/polym14061150 - 13 Mar 2022

Cited by 23 | Viewed by 2325

Abstract

This is a study of concept on the initial application for wood adhesives totally biosourced from the covalent reaction between soy protein isolate (SPI) and a commercial flavonoid tannin, namely quebracho tannin. The adhesive is composed exclusively of the two vegetable biomaterials mentioned and thus is totally biosourced and non-toxic, as tannin has been classified as being not at all toxic by the European Commission REACH program. The pre-reaction between the two yielded the best plywood bonding results when limited to a temperature of 40 °C, final cross-linking being achieved during the plywood higher temperature hot pressing procedure, as for any other thermosetting adhesive. Pre-reaction at higher temperatures, namely 60 °C and 80 °C, achieved extensive premature cross-linking that lost any activity to cross-link further when hot pressed for preparing plywood. The reaction was followed by thermomechanical analysis, by matrix assisted laser desorption ionization time of flight (MALDI ToF) mass spectrometry, and by plywood shear strength tested dry, after a 24 h cold water soak and 1 h in boiling water. The adhesive of this approach lends itself to be further reinforced by the multitude of approaches on soy resins already developed by several other research groups. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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Open AccessArticle

Graphene Oxide Functionalized Cottonseed-Lignin Resin with Enhanced Wet Adhesion for Woody Composites Application

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Polymers 2022, 14(1), 1; https://doi.org/10.3390/polym14010001 - 21 Dec 2021

Cited by 4 | Viewed by 1764

Abstract

With rising interior air pollution, health, and food shortage concerns, wood adhesives derived from non-food sustainable materials have therefore attracted considerable attention. Here we developed an eco-friendly cottonseed-lignin adhesive consisting of non-food defatted cottonseed flour (DCF), alkali lignin (AL), and graphene oxide (GO). The cation-π interaction, and hydrogen and covalent bonds between AL@GO and DCF collectively enhanced the cross-linking structure of the cured cottonseed-lignin adhesive, based on the Fourier-transform infrared spectroscopy, thermogravimetric analyses, scanning electron microscopy, and sol-gel tests. The high performance of the developed cottonseed-lignin adhesive was evidenced by its increased wet/dry shear strength and decreased rheological properties before curing and improved thermal stability and decreased soluble substances after curing. Particularly, the highest wet shear strength of poplar plywood bonded with cottonseed-lignin adhesive was 1.08 MPa, which increased by 74.2 and 54.3% as compared to the control and requirement of the Chinese standard GB/T 9846-2015 for interior plywood (≥0.7 MPa), respectively. The technology and resultant adhesives showed great potential in the preparation of green woody composites for many applications. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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Open AccessArticle

A Comparison among Lignin Modification Methods on the Properties of Lignin–Phenol–Formaldehyde Resin as Wood Adhesive

Hamed Younesi-Kordkheili

and

Antonio Pizzi

Polymers 2021, 13(20), 3502; https://doi.org/10.3390/polym13203502 - 12 Oct 2021

Cited by 16 | Viewed by 2598

Abstract

The research aim of this work is to determine the influence of lignin modification methods on lignin–phenol–formaldehyde (LPF) adhesive properties. Thus, glyoxal (G), phenol (P), ionic liquid (IL), and maleic anhydride (MA) were used to modify lignin. The modified lignins were used for phenol substitution (50 wt%) in phenol–formaldehyde adhesives. The prepared resins were then used for the preparation of wood particleboard. These LPF resins were characterized physicochemically, namely by using standard methods to determine gel time, solids content, density, and viscosity, thus the physicochemical properties of the LPF resins synthesized. The panels dimensional stability, formaldehyde emission, bending modulus, bending strength, and internal bond (IB) strength were also measured. MA-modified lignin showed by differential scanning calorimetry (DSC) the lowest temperature of curing than the resins with non-modified lignin and modified with IL, phenolared lignin, and glyoxal. LPF resins with lignin treated with maleic anhydride presented a shorter gel time, higher viscosity, and solids content than the resins with other lignin modifications. Equally, the particleboard panels prepared with LPF resins with maleic anhydride or with ionic liquid had the lowest formaldehyde emission and the highest mechanical strength among all the synthesized resins. The dimensional stability of all panels bonded with modified lignin LPF resins presented no difference of any significance. Full article

(This article belongs to the Special Issue Renewable Polymeric Adhesives II)

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