Solid-Phase Molecular Self-Assembly Enabled Glue-Free Antifatigue Laminate Programmable Materials.

Repeated programmability has emerged as a desired property in smart device engineering, but the programmability will fatigue upon repeated applications due to the unmatched mechanical property between the layer materials and the polymeric glue that is required to integrate the two individual oriented layers. It is reported here that glue-free antifatigue programmable laminate materials can be made with films resulted from solid-phase molecular self-assembly (SPMSA). The SPMSA films are created by squeezing the precipitates of oppositely charged polyelectrolytes and DTAB with a noodle machine, where the hydrophobic DTAB molecules self-assembled into wormlike micelles and oriented along the squeezing direction. The surface molecules in this film are endowed with sufficient mobility in the presence of hydration water, so that two such films are able to be pressed into a laminate material owing to the hydrophobic and electrostatic interactions between the molecules on the two adjacent surfaces. As the water evaporated gradually, the left laminate materials are glue-free with the same composition. When many of such films are integrated with specific designs, complicated shape programming is able to be achieved, and the programmability is reversible without fatigue. The current strategy is envisioned as a potent intriguing pathway leading to advanced programable materials.

Unprecedented Nonflammable Organic Adhesives Leading to Fireproof Wood Products.

We report an excellent water-based inflammable organic wood adhesive that is able to protect wood products from burning by generating inflammable gases, a porous thick char layer, and radicals that consume the oxygen and hydrogen radicals required in the burning process. The organic adhesive is obtained by the formation of hard supramolecular phases composed of high-density flame-retardant N and P elements through hydrogen bonding and acid-base interaction between the phytic acid and branched polyethylenimine (b-PEI). The phytic acid molecules are packed densely in the framework of the flexible b-PEI so that a porous char layer that would reduce heat conduction can be formed as the adhesive is heated. Together with the formation of inflammable NH3 gas to dilute the oxygen concentration and a PO• radical to capture the H• and O• radicals, the adhesive-treated wood product displays an extremely high limited oxygen index of 100% and a negligible heat release rate, total heat release, and total smoke release. The current flame-retardant water-based organic adhesive is so far the best adhesive for green and safe wood products from burning.

Folic Acid-Based Coacervate Leading to a Double-Sided Tape for Adhesion of Diverse Wet and Dry Substrates.

Adhesives are crucial both in nature and in diversified artificial fields, and developing environment-friendly adhesives with economic procedures remains a great challenge. We report that folic acid-based coacervates can be a new category of excellent adhesives for all kinds of surfaces with long-lasting adhesiveness. Aided by the electrostatic interaction between the π-π stacked folic acid quartets and polycations, the resultant coacervates are able to interact with diversified substrates via a polyvalent hydrogen bond, coordination, and electrostatic interactions. The adhesivity to wood is superior to the strong commercial glues, but without releasing any toxic components. Upon evaporating water, the coacervate can be casted into a non-adhesive flexible self-supporting film, which restores the adhesive coacervate immediately on contacting water with original adhesive ability. In this way, the coacervate can be facilely tailored into a double-sided tape (DST), which is convenient for storage and application under ambient conditions. Given its excellent adhesive performance, release of nontoxic gases, and convenience in storage and application, the folic acid-based DST is very promising as a new adhesive material.

Green Wood Adhesives from One-Pot Coacervation of Folic Acid and Branched Poly(ethylene imine).

Adhesives are extensively used in furniture manufacture, and most currently utilized furniture glues are formaldehyde-based chemicals, which emit formaldehyde throughout the entire life of the furniture. With increasing concerns about formaldehyde emission effects on human health, formaldehyde-free and environmentally friendly wood adhesives from bio-based resources are highly desired. In this study, we developed an eco-friendly, high-strength, and water-based wood adhesive from one-pot coacervation of the hierarchical self-assembly of folic acid (FA, a biomolecule, vitamin B9) with a commercially available biocompatible polymer-branched poly(ethylene imine) (b-PEI). The coacervation is caused by multiple hydrogen bonds between b-PEI and the stacks of FA quartets, which demonstrates a continuous robust 3D network, thus realizing adhesion and cohesion behaviors. This coacervate has the strongest adhesion toward wood compared with other substrates. The long-lasting shear bonding strength is up to 3.68 MPa, which is much higher than that of commercial super glue, but without releasing any toxic components. Since all the fabrication and application processes are under ambient conditions without any heating and high-pressure procedures, this work provides a facile yet powerful strategy to develop formaldehyde-free, eco-friendly, and high-performance bio-based waterborne adhesives for wood bonding.