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High-concentration graphene slurries are highly needed in the manufacturing of many functional materials, such as for printing or spin coating, which typically require a high solid content in the work window as shown in Figure a. The logarithmic plot of graphene content (c) versus storage/loss modulus shows that at pH = 14, the critical gel concentration (cg) of the graphene slurry is ~1.25 wt%. Below this cg, flocculated graphene sheets form separate microscale aggregates. The system exhibits liquid-like behavior, where the loss modulus (G″) is greater than the storage modulus (G') within the measured frequency range. Beyond cg, G' exceeds G″, and the slurry behaves like an elastic gel.
Here, we have manufactured various graphene aerogel structures using high-concentration slurries in the elastic gel region for 3D printing, as shown in Figure d. To the best of our knowledge, this is the first demonstration of aqueous-phase 3D printing of exfoliated graphene. Previous research on graphene aerogels relied on sol-gel chemistry, which poses challenges for large-scale production. The printed aerogels are macroporous (Figures e, f) and exhibit good mechanical strength.
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