Mid-temperature deep removal of hydrogen sulfide on rare earth (RE = Ce, La, Sm, Gd) doped ZnO supported on KIT-6: Effect of RE dopants and interaction between active phase and support matrix

Abstract

Rare earth oxides (RE=Ce, La, Sm and Gd) doped ZnO supported on KIT-6 sorbents (RE-ZnO/KIT-6) were synthesized by sol-gel method and their performance for deep removal of H2S (bellow 0.1 ppmv) from gas stream at medium temperature was tested. The RE dopants (except Ce) significantly enhance the deep desulfurization capacity of ZnO/KIT-6 sorbent and maintained higher sulfur uptake capacities upon multiple cycles of regeneration by a simple thermal oxidation in 10v% of O2 in N2 atmosphere. The results of SAXS, XRD, N2 physisorption, TEM, FIIR, and XPS implied that the KIT-6 structure of loading metal oxides remained intact. It was found that RE could hinder the ZnO crystal ripening during calcination resulted in smaller ZnO particles, enhance the interaction of ZnO and silica matrix to improve the dispersion of active phase on KIT-6. Furthermore, by increasing the outlayer electron density of Zn atom and oxygen transfer ability, the synergistic effect considered to be favorable for RE-ZnO/KIT-6 sulfidation. Even though the performance of improving ZnO dispersion was weaker than that of Sm and Gd, La-ZnO/KIT-6 performs the best deep desulfurizers by changing the surface chemical atmosphere for ZnO. Steam in the gas stream inhibited the capture of H2S by ZnO in the sorbents, in the case of La-ZnO/KIT-6, the steam content should control as lower as 5v% to ensure the desulfurization efficiency and precision.