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The integrated CO 2 capture and utilization employs chemical looping approach for suppressing the equilibrium limitations of traditional gas-solid catalytic reactions, enabling efficient conversion of dilute CO 2 into high-value fuels with minimal energy consumption. However, the diminishing cyclic activity of dual-functional materials poses significant challenges to their industrial application. Herein, we tailored a series of magnesium-calcium materials, the influence of coordinated metals on the cyclic performance were quantitatively investigated. Notably, Fe 2 Ni 2 Ce 2 Mg 5 Ca 20 CO 3 achieves a cumulative CO yield of 121.0 mmol/g over 15 cycles at 650°C, with a maximum CO yield of 8.3 mmol/g per cycle and 99.0% CO selectivity, and its CO 2 capture capacity remains stable at 10.6 mmol/g over 37 adsorption/desorption cycles. Experimental results indicate that lattice phase separation is a fundamental mechanism underlying the decline in cyclic activity. The strategic incorporation of transition metal intermediates promotes the formation of dispersed metal-carbonate interfaces, providing surface hydrogenation sites and accelerating the lattice decomposition and reconstruction of CO 3 * within a dispersed lattice. This modification mitigates the adsorption/catalytic lattice phase separation, boosts metal migration and deoxygenation activity for cyclic nanoparticle construction. The findings offer valuable strategies for designing highly efficient and stable DFMs in CO 2 capture and utilization.
Cao et al. (Wed,) studied this question.