Synergistic Chemical Looping Process Coupling Natural Gas Conversion and NOx Purification

We present a novel low-temperature chemical looping combustion scheme for simultaneous natural gas conversion into a sequestration-ready CO2 stream and NOx 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 NOx-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 NOx purification performance at different flue gas flow rates. The operating temperatures of the reactors are selected based on NOx- 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 degrees 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 NOx conversion. For the autothermal analysis, the CH4 reactor operates adiabatically, while the NOx reactor operates isothermally. Comparative studies with the conventional NOx 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 NOx 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 NOx emissions.