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A tunable and efficient strategy was adopted to synthesize highly porous nano-structured CuO−carbonized composites (CuxO@C) using Cu3(BTC)2 as a sacrificial template. The as-synthesized CuO nanocomposites exhibited hollow octahedral structures, a large surface area (89.837 m2 g−1) and a high proportion of Cu2O active sites distributed on a carbon frame. Based on DFT calculations, both the Cu atoms on the surface (CuS) and oxygen vacancy (OV) exhibited strong chemical reactivity. On the perfect CuO (111), the CuS transferred charge to O atoms on the surface and SO2 molecules. A strong adsorption energy (−1.41 eV) indicated the existence of the chemisorption process. On the oxygen-deficient CuO (111), the O2 preferably adsorbed on OV and then formed SO3 by bonding with SO2, followed by the cleavage of the O−O bond. Furthermore, the CuO nanocomposites exhibited an excellent ratio of S/Cu in SO2 removal experiments compared with CuO nanoparticles produced by coprecipitation. [ABSTRACT FROM AUTHOR]

A highly efficient desulfurizer is derived from a sacrificial Cu-based metal-organic framework (MOF) template, which is loaded on low-cost activated semi-cokes. The carbonized composite possesses highly-dispersed copper oxide nanoparticles (Cu 2 O/CuO) as active sites, which are distributed on MOF-derived carbon octahedra and activated semi-cokes. With an ultralow surface loading of 0.19 at% Cu and a high proportion of Cu+, the optimized sample shows an excellent breakthrough time of 822 min and SO 2 adsorption capacity of 233.11 mg/g with a steady SO 2 removal efficiency of 100%, which is superior to previously reported coke-base desulfurizers in literature. Meanwhile, the best-performed sample shows stability and reversibility for SO 2 removal during 10 desulfurization−regeneration cycles. The excellent SO 2 removal performance can be attributed to a well-developed porous structure and highly-dispersed copper oxide active sites due to the utilization of both sacrificial MOF template and activated semi-coke. [Display omitted] [ABSTRACT FROM AUTHOR]