Abstract
In the realm of environment and energy sectors, the strategic designing of adsorbents utilizing active Cu1+-based composite materials stands as a pivotal initiative for effective CO removal. However, the commercial viability of these composites was hindered by oxidation tendency of active Cu1+ species during ambient storage, leading to a gradual decline in activity. Concurrently, selectivity constraints pose challenges to the practical utility of Cu1+-based CO adsorbents. In this study, a synergistic dual inorganic–organic stabilization system was introduced to address inherent stabilization and selectivity constraints. The SnO2-chitosan coupled stabilizer was employed to exploit dual chemical stabilization interactions which involved synergistic redox behavior within active Cu2O-SnO2 interface stemming from strong Sn-O interaction in contrast to that of Cu–O and coordinated chelation facilitated by the unsaturated nitrogen sourced from chitosan in conjunction with Cu1+ species. These mechanisms effectively preserved the oxidative susceptibility of active Cu1+ ions and impeded their gradual deactivation. The stable structural formation and complexation effects were validated through TEM, XPS, and in-situ FTIR analyses. Remarkably, incorporating a small quantity of SnO2 with organic chitosan stabilizer within the composite maintained ∼ 99 % stability of the initial adsorption uptake (∼24 cm3/g) even after 30-day storage under ambient conditions, surpassing the adsorption stability performance of the adsorption composite with only organic chitosan stabilizer. Furthermore, inclusion of SnO2 attenuated the surface basicity stemming from nitrogen-doping which favors the CO2 adsorption over CO, and due to the enhanced surface acidity as confirmed through NH3-TPD and in-situ FTIR analyses, a higher CO selectivity of 7.1 over CO2 was achieved. In conclusion, this study highlighted the advantageous potential of an inorganic–organic stabilizing system, specifically SnO2-chitosan combination, offering a viable approach to address stability and selectivity challenges associated with the Cu1+-based CO adsorption, presenting a viable pathway for the development of practical CO adsorbents.
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