We present a novel low-temperature chemical looping combustion
scheme for simultaneous natural gas conversion into a sequestration-ready
CO2 stream and NO
x
purification.
The scheme employs nickel oxide (NiO) supported on ZrO2 as the oxygen carrier. In the process, CH4 reduces the
oxidized carrier to Ni/ZrO2 in a co-current moving bed
reactor, which is then oxidized back to NiO/ZrO2 by the
NO
x
-laden flue gas in a fluidized bed
reactor, completing the oxygen carrier loop. Thermodynamic studies
demonstrate that the presence of CO2 does not significantly
affect NO
x
purification performance at
different flue gas flow rates. The operating temperatures of the reactors
are selected based on NO
x
-temperature
programmed oxidation (TPO) and CH4-temperature programmed
reduction (TPR) experiments. Results show that the process can optimally
operate at temperatures close to the combustion plants’ flue
gas temperature of 400–500 °C, reducing the need for hot
utilities. The study conducts comprehensive isothermal and autothermal
analyses of the process to evaluate the effects of temperature and
carrier flow rate on CH4 conversion, CO2 selectivity,
carbon deposition, and NO
x
conversion.
For the autothermal analysis, the CH4 reactor operates
adiabatically, while the NO
x
reactor operates
isothermally. Comparative studies with the conventional NO
x
selective catalytic reduction (SCR) process
indicate an exergy efficiency and effective thermal efficiency (ETE)
improvement of 9 and 18 percentage points, respectively. The findings
suggest that this low-temperature chemical looping process is a promising
solution for flue gas NO
x
treatment, utilizing
cheaper natural gas as the reductant and eliminating environmental
concerns, such as ammonia or urea slippage. Overall, this study contributes
to the development of more efficient and sustainable methods for reducing
NO
x
emissions.