This paper is a study of the composition dynamics of Liesegang band strata of Co(OH)2 and Ni(OH)2 from NH4OH, with redissolution by complex formation with ammonia. At a fixed time, the cobalt hydroxide composition was found to exhibit a random variation with band number, yet within a general overall decrease. The decrease with band number becomes more pronounced as the initial concentrations of Co2+ and Ni2+ get closer to each other. At equal concentrations, periodic oscillations in Co(OH)2 composition appear over consecutive bands. The time evolution of the total Co(OH)2 mass percent (over the entire pattern of strata) passes through a maximum. The dynamics of this complex system has been simulated by theoretical calculations using the model of Müller and Polezhaev, modified by Al-Ghoul and Sultan in a series of two papers in J. Phys. Chem. A; the present paper is the third in the series. The simulations capture the essential features of the experimentally observed dynamics.

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Liesegang banding is the display of rhythmic strata of precipitate as co-precipitate ions interdiffuse in a gel medium. Complex periodic patterns as well as aperiodic structures could emerge, notably in systems where more than one salt is precipitated. The use of three cations (Co2+) Ni2+, and Mg2+) in the banded precipitation of their hydroxides resulted in an unusual pattern with a consistently increasing rhythmicity. A periodic structure marked by the succession of band multiplets with increasing number of bands (from singlets to doublets to triplets to quadruplets, consistently) was observed. Such rhythmic patterns are obtained as the initial Mg2+ concentration ([Mg2+]0), chosen as a control parameter, increases through a critical value. At high [Mg2+]0, the trend breaks after a long time elapses. Two types of bifurcation are therefore experienced by such a system: concentration bifurcation and diffusive (time/space) bifurcation. The dynamics is elucidated on the basis of an analysis of the bands in certain groups, and gel regions between these groups, as well as between group blocs (here, a bloc denotes a succession of multiplet groups, with repetitively the same number of bands). Finally, similarities between our system and naturally occurring rhythmic patterns are emphasized and discussed.

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