Abstract:
The photocatalytic reduction of carbon dioxide (CO sub(2)) into multi-electron carbon products remains challenging due to the inherent stability of CO sub(2) and slow multi-electron transfer kinetics. Here in, we synthesized a hybrid material, cesium copper halide (Cs sub(3)Cu sub(2)I sub(5)) intercalated onto two-dimensional (2D) cobalt-based zeolite framework (ZIF-9-III) nanosheets (denoted as Cs sub(3)Cu sub(2)I sub(5)@ZIF-1) through a simple mechanochemical grinding. The synergy in the hybrid effectively reduces CO sub(2) to carbon monoxide (CO) at 110 Mu mol/g/h and methane at 5 Mu mol/g/h with high selectivity, suppressing hydrogen evolution. Further, we have investigated additional Cs sub(3)Cu sub(2)I sub(5)@ZIF hybrids with varying ZIF-9-III amounts, confirming their selective CO sub(2) reduction to methane over hydrogen. Density functional theory (DFT) calculations reveal a non-covalent interaction between Cs sub(3)Cu sub(2)I sub(5) and ZIF-9-III, with electron transfer suggesting potential for improved photocatalysis.
