We designed a diffusion-induced gelation process for GO colloids in a static state to prepare bulk freestanding GO gels as reflecting coagulation behavior (Fig. 2, A and B). Open-ended glass tubes (inner diameter, 14 mm) were used as a mold. In a typical process, one side of the tube was closed with a dialysis membrane (molecular weight cutoff, 6000 to 8000; Spectra Dialysis Membrane), and 2 ml of the GO dispersion (0.5 wt %) was injected into the tube through the other side. Then, the tube was submerged in a beaker containing 50 ml of the coagulation solution, and the level of the GO dispersion was adjusted to be equivalent to that of the coagulation solution. The membrane was semipermeable with an average pore size small enough to prevent infiltration of GO sheets (average diameter, 1.7 μm) and therefore mediated ion diffusion at the interface only toward the GO dispersion (Fig. 2B). Once the tube was submerged, the sol-gel transition occurred, and the GO dispersion was fully converted to a gel after 12 hours (fig. S6A). The freestanding GO hydrogel was separated from the tube and washed by soaking in 50 ml of DIW. The DIW was replaced more than five times at fixed time intervals of 6 hours.

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