The HSC Chemistry software (version 6.0, Outotec Technologies) was used in this study to calculate the Gibbs free energy, enthalpy, and thermodynamic equilibrium of related reactions according to the criterion of Gibbs free energy minimization. On the basis of these thermodynamic calculations, the energy consumption for CO2 utilization (ECO2, kJ molCO21) and fuel requirement for syngas production (XCH4, molCH4 molsyn1) of the proposed CaL methane reforming process can be determined via Eqs. 3 and 4, respectively, once an initial amount of reactants and the corresponding carbonation and calcination temperatures are specified.ECO2(T1,T2)=EReaction i+EReactant knCO21[n]CO21[n]CO22[n]CaCO32(3)XCH4(T1,T2)=(EReaction i+EReactant k)/HHVCH4+nCH42[n]CH42[n]H22+[n]CO2(4)where EReaction i (kJ) and EReactant k (kJ) represent the energy required to drive the chemical reaction i and heat the related reactant k to the carbonation temperature (T1, K) or calcination temperature (T2, K), respectively. nk1 (mol) and [n]k1 (mol) represent the initial and equilibrium amounts of the reaction species k, respectively, at the carbonation step, while nk2 (mol) and [n]k2 (mol) represent those at the calcination step. HHVCH4 represents the high heat value of methane (kJ mol−1).

The terms EReaction i and EReactant k in the above equations can be determined via Eqs. 5 and 6, respectively.EReaction i=(nk[n]k)ΔHi(5)EReactant k=nkCPk(T)dT(6)where ΔHi (kJ mol−1) and CPk (kJ mol−1 K−1) represent the enthalpy of reaction i and the heat capacity of reactant k, respectively.

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