From hydrodynamic plumes to chemical gardens: the concentration-dependent onset of tube formation.

Many inorganic precipitation reactions self-organize macroscopic tubes known as chemical gardens. We study the nonequilibrium formation of these structures by injecting aqueous sodium sulfide solution into a reservoir of iron(II) chloride solution. Our experiments reveal a distinct, concentration-dependent transition from convective plumes of reaction-induced, colloidal particles to mechanically connected, hollow tubes. The transition concentration (0.1 mol/L) is widely independent of the injection rate and causes a discontinuous change from the radius of the plume stalk to the radius of the tube. In addition, tubes have lower growth speeds than plumes. At the transition concentration, one observes the initial formation of a plume followed by the growth of a mechanically weak tube around a jet of upward-moving precipitation particles. We find that the plumes' morphology and geometric scaling are similar to that of laminar starting plumes in nonreactive systems. The characterization of dried tubes by X-ray diffraction indicates the presence of greigite and lepidocrocite.