Recently, a novel two-stage reactor
configuration for packed bed
chemical-looping combustion (CLC) has been proposed and studied by
numerical simulations. This two-stage CLC consists of two pressurized
packed bed reactors connected in series, where the first bed contains
an oxygen carrier material which is reactive at relatively low temperatures
(450 °C) such as CuO/Cu, while the second bed contains an oxygen
carrier which is resistant to relatively high temperatures (typically
1200 °C) such as NiO/Ni. In this work, this two-stage CLC concept
has been experimentally demonstrated using CuO/Al2O3 and NiO/CaAl2O4 as bed materials in
a high-pressure, high-temperature packed bed reactor. The influence
of the operating conditions has been examined, and a validated reactor
model has been used to scale up the process to industrial scale. The
two-stage CLC concept is successfully demonstrated with a maximum
temperature of 839 °C in the second bed. The operating pressure,
the throughput during the reduction cycle, and the fuel concentrations
have been found to result in small or negligible influences on the
maximum temperature rise. This means that they do not affect the TS-CLC
performance as long as the cycle time is adopted such that the heat
produced in the first reactor bed is exactly transferred to the second
bed. It has also been demonstrated that operation at higher pressures
(to reach a higher overall process efficiency) does not affect the
performance of the TS-CLC reactor. However, the fuel type (H2, syngas, CO, or CH4) strongly influences the temperature
increase in the reactor, since it influences to what extent the oxygen
carriers can be reduced. The experimental results could be well described
by a one-dimensional packed bed reactor model provided that the extent
of heat losses and the response time of the thermocouples are properly
taken into account. The validated reactor model shows that the desired
gas flow rate at 1200 °C can indeed be produced after some small
changes in the operating conditions and the active weight content
of the oxygen carriers. Therefore, TS-CLC can be regarded as a feasible
technology for power production with inherent CO2 capture
with high LHV efficiency.