Facile and Versatile Sol-Gel Strategy for the Preparation of a High-Loaded ZnO/SiO2 Adsorbent for Room-Temperature H2S Removal

Langmuir. 2019 Jun 18;35(24):7759-7768. doi: 10.1021/acs.langmuir.9b00853. Epub 2019 Jun 7.

Abstract

Preparation of well-dispersed ZnO nanograins is necessary to improve their reactivity toward room-temperature H2S removal. However, the challenge to design such a ZnO-based adsorbent with high ZnO loading is yet to be fulfilled. Herein, a facile sol-gel strategy is reported for the preparation of ZnO/SiO2 adsorbents for efficient H2S removal, by innovating a gel-drying method and simultaneously controlling ZnO grain formation through optimizing the molar ratio of ethylene glycol (EG)/nitrates in its precursors. The fabricated adsorbent embedded well-dispersed ZnO nanograins, of approximately 10-15 nm, into a SiO2 matrix (57 wt % ZnO loading) and thus yielded a high H2S removal capacity of 108.9 mg S/g sorbent. Therein, EG was used as a modifier for inhibiting the formation of a denser SiO2 network during the gel drying process and was used as a fuel for promoting the decomposition of nitrates and increasing the surface area of the composites in the subsequent calcination. Modulating the molar ratio of EG/nitrates ≤ 2 in precursors or traditional drying of the gel in an oven should be avoided because these would lead to the oxidation of EG by metallic nitrates and form carboxylate complexes during the gel-drying process. Although the produced ZnO grains had a very small size of less than 5 nm, a layer of monodentate ZnCO3 impurity was formed on the ZnO surface, which will drastically decrease the reactivity of ZnO toward H2S. According to the encouraging results from CuO and Co3O4, this strategy has proved to be versatile for the preparation of other metal oxide/SiO2 adsorbents.