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Polymers That Heal Themselves

Materials Science: Two-stage process of gelation and polymerization repairs holes as big as 9 mm in polymers

by Celia Henry Arnaud
May 8, 2014 | A version of this story appeared in Volume 92, Issue 19

Credit: Nathan Bajandas/UIUC
In this time sequence of images, a 4.75-mm hole in a polymer is repaired by mixing two solutions (dyed blue and red) that react to form a gel scaffold and a polymerized solid.
Overhead view of time sequence of polymer repair.
Credit: Nathan Bajandas/UIUC
In this time sequence of images, a 4.75-mm hole in a polymer is repaired by mixing two solutions (dyed blue and red) that react to form a gel scaffold and a polymerized solid.

Biological systems can heal themselves. That’s not usually true for materials made with synthetic polymers. Although researchers have previously reported self-healing polymers, such repairs have been limited to microscopic defects and cracks.

A new system, devised by researchers at the University of Illinois, Urbana-Champaign, enables the self-healing in polymers of holes as big as 9 mm (Science 2014, DOI: 10.1126/science.1251135). Aerospace engineer Scott R. White, chemist Jeffrey S. Moore, materials scientist Nancy R. Sottos, and coworkers developed a two-stage gelation and polymerization process to carry out these repairs. The researchers envision using the process in structural materials and other plastics prone to impact damage.

The process depends upon channels embedded in the polymer. Those channels contain solutions that remain segregated until they are needed for repairs. One channel contains a solution of a gelator, a catalyst, and a promoter. Another channel contains a solution of another gelator and an initiator. The monomers needed for the reaction are divided between the channels. Damage to the polymer breaks open the channels, releasing the solutions and allowing them to mix.

The two gelators form a cross-linked network that turns the solution into a gel. The gelation continues until the hole is filled with a gel scaffold. That scaffold then polymerizes into a solid. These two stages occur on different timescales—seconds to minutes for the gel formation and hours for the polymerization.

“We’re able to tune the system so the gel time is relatively fast but the polymerization time is much slower,” Sottos says. “I don’t think we’ve really hit the optimum yet for the gel formation versus polymerization, but the polymerization time should come much later than the gel or you’ll never get the full scaffold to form.”

The researchers demonstrated damage repair with two different types of polymers—a methacrylate-based polymer and a thiolene-based polymer. In one example, they repaired an open cylindrical hole. In a more realistic example, they repaired materials that they had crushed and punctured with a metal striker.

So far, the method is limited to damage holes smaller than about 9 mm. “Currently, the worst enemy of the concept appears to be gravity,” says Fred Wudl, a materials chemist at the University of California, Santa Barbara. If the hole is too big, gravity pulls unreacted fluid out of the damage zone before it has a chance to gel. “One wonders what this inventive group has up their sleeve to emasculate gravity.”


“This two-stage approach has considerable design versatility,” says Richard P. Wool, a professor of chemical and biomolecular engineering at the University of Delaware. “Many future variants could be visualized, such as self-assembling scaffolds, even fibers in composites and reactive nanostructures.”


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