Integrated CO2 Capture and Utilization by Combining Calcium Looping with CH4 Reforming Processes: A Thermodynamic and Exergetic Approach

Abstract

This study investigates a novel concept to coproduce high-purity H2 and syngas, which couples steam methane reforming with CaO carbonation to capture the generated CO2 and dry reforming of methane with CaCO3 calcination to directly utilize the captured CO2. The thermodynamic equilibrium of the reactive calcination stage was evaluated using Aspen Plus via a parametric analysis of various operating conditions, including the temperature, pressure, and CH4/CaCO3 molar ratio. Introducing a CH4 feed in the calcination stage promoted the driving force and completion of CaCO3 decomposition at lower temperatures (∼700 °C) compared to applying an inert flow, as a result of in situ CO2 conversion. A conceptual process design was investigated that employs a system of two moving bed reactors to produce nearly equivalent volumetric flows of pure H2 and a syngas stream with a H2/CO molar ratio close to 1. A solar reactor was examined for the reactive calcination step to cover the energy requirements of endothermic CaCO3 decomposition and dry reforming. The overall exergy efficiency of the process was found equal to ∼75.9%, a value ∼4.0 and ∼8.0% higher compared to sorption-enhanced reforming with oxy-fuel and solar calciner, respectively, without direct utilization of the captured CO2