This study systematically investigates the pressure fluctuation in the riser of a dual interconnected circulating fluidized bed (CFB) representing a 10 kW th cold-flow model (CFM) of a chemical-looping combustion (CLC) system. Specifically, a single-species system (SSS) and a binary-mixtures system (BMS) of particles with different sizes and densities were utilized. The pressure fluctuation was analyzed using the fast Fourier transform (FFT) method. The effect of introducing a second particle, changing the inventory, composition (i.e., 5, 10 to 20 wt.%), particle size ratio, and fluidization velocity were investigated. For typical SSS experiments, the results were similar to those scarcely reported in the literature, where the pressure fluctuation intensity was influenced by varying the initial operating conditions. The pressure fluctuations of BMS were investigated in detail and compared with those obtained from SSS experiments. BMS exhibited different behaviour; it had intense pressure fluctuation in the air reactor and in the riser when compared to SSS experiments. The standard deviation (SD) of the pressure fluctuation was found to be influenced by the fluidization regime and initial operating conditions, while the power spectrum density (PSD) values were more sensitive to the presence of the particles with the higher terminal velocity in the binary mixture.Processes 2019, 7, 890 2 of 25 beds are complex, primarily determined by the combined effects of solids' behaviour and bubbles' characteristics in terms of development, movement, and burst. The application of chemical-looping combustion (CLC) lies between these two points, i.e., it is both part of the chemical engineering application and in energy conversion and steam production.It has been well documented that utilizing a mixture of metal oxides significantly improves the oxygen storage capacity of oxygen carrier particles in CLC systems that consist of dual interconnected circulating fluidized bed (CFB) [3,4]. This mixture of oxygen carrier was used as a single particles carrier containing both ingredients. However, other systems utilize a binary-mixture system (BMS) as two separate species that differ in sizes and/or densities in bubbling fluidized beds [5][6][7][8][9][10][11][12][13][14][15][16], and in a single-column fluidized bed [17][18][19][20][21]. Utilizing a BMS that differs in size and/or density will raise a number of operational uncertainties associated with the mixing/segregation of particles and the hydrodynamics of these complex systems. Mixing and segregation of binary solids that differ in both size and density have been investigated previously, where an operating map was developed to avoid any type of segregation (i.e., local or components segregation) in CLC systems [22][23][24]. The hydrodynamics of BMS in a dual interconnected CFB are yet to be investigated extensively. Specifically, the effects of parameters including particle size and density, mixture composition, total solids inventory (TSI) on the pressure profile, solids holdup...