Decreasing
the reduction temperature of an oxygen carrier is the key to reduce
energy consumption further and avoid the operational difficulties
of chemical looping air separation (CLAS). The copper manganese composite
oxygen carrier with zirconia as an inert binder, which has a relatively
low temperature of oxygen uncoupling, was developed. In the packed-bed
reactor, effects of several important operating parameters, viz.,
the feed gas rate, temperature, and inlet oxygen concentration, on
the separation reactivity were discussed. At higher reaction temperatures,
the reduction reactivity increases but the oxidation reactivity decreases.
In comparison to a copper oxygen carrier, the equilibrium oxygen concentration
of the copper manganese oxygen carrier is greatly enhanced. High gas
flow rates can accelerate the separation reaction. In the reduction
step, a lower oxygen concentration leads to a higher reduction reactivity.
In the oxidation step, the higher oxidation reactivity requires higher
oxygen concentrations. The oxygen uncoupling kinetics was determined
by the lnln kinetic method. The separation activation energy was determined
at 162.95 kJ mol–1, and the most likely mechanism
function is the unreacted shrinking core model (R
2). The main compositions in fresh and oxidized composite
oxygen carriers are Cu
x
Mn3–x
O4 and ZrO2. After reduction,
the active phase compositions are transformed into Cu
x
Mn2–x
O2. The inert phase of ZrO2 is stable during the redox reaction.
The repeated separation capability of the composite oxygen carrier
over 20 consecutive redox cycles is high.