Evaluation of CuAl2O4 as an Oxygen Carrier in Chemical-Looping Combustion

The chemical-looping combustion (CLC) process is a novel solution for efficient combustion with intrinsic separation of carbon dioxide. The process uses a metal oxide as an oxygen carrier to transfer oxygen from an air to a fuel reactor where the fuel, or gasification products of the fuel, reacts with the solid oxygen carrier. In this work, copper(II) aluminate (CuAl 2 O 4 ) was assessed as a potential oxygen carrier using methane as fuel. The carrier particles were produced by freeze–granulation and calcined at 1050 °C for a duration of 6 h. The chemical-looping characteristics were evaluated in a laboratory-scale fluidized-bed reactor in the temperature range of 900–950 °C during 45 alternating redox cycles. The oxygen carrier exhibited reproducible and stable reactivity behavior in this temperature range. Neither agglomeration nor defluidization was noticed in any of the cycles carried out at 900–925 °C. However, after reactivity tests at 950 °C, soft agglomeration and particle fragmentation were observed. Systematic phase analysis of the Cu–Al–O system during the redox cycle was carried out as a function of duration of reduction and oxygen concentration during the oxidation period. It was found that the CuAl 2 O 4 is reduced to copper(I) aluminate (CuAlO 2; delafossite), Cu 2 O, and elemental Cu. The CuAlO 2 phase is characterized by slow kinetics for oxidation into CuO and CuAl 2 O 4 . Despite this kinetic limitation, complete conversion of methane with reproducible reactivity of the oxygen carrier is achieved. Thus, CuAl 2 O 4 could be a potential oxygen carrier for chemical-looping combustion.