JiuJu Magnetism Industry News] Preparation method of LaCoO3 chalcogenide material and its catalytic degradation effect on formaldehyde wastewater

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Formaldehyde (HCHO) is a widespread water-soluble toxic pollutant, which mainly originates from industrial production emissions, volatilization of building and decoration materials, and the release of daily necessities. This compound is strongly carcinogenic and biotoxic, which will not only cause serious damage to the human respiratory system and immune system, but also destroy the ecological balance of the water body. Therefore, the development of efficient formaldehyde removal technology is of great significance for the protection of human health and the maintenance of ecosystem stability. The existing formaldehyde degradation methods mainly include adsorption technology, biodegradation method and catalytic oxidation method, among which catalytic oxidation method has become the key direction of the current research due to its advantages of complete degradation and no secondary pollution.

Calcite-type oxides (ABO₃), with unique crystal structures, excellent electronic conductivity and stable catalytic activity, have made remarkable progress in multiphase catalysis such as CO oxidation and volatile organic compound degradation. As a typical chalcogenide material, lanthanum cobalt oxide (LaCoO₃) has a potential oxidation catalytic ability due to the valence tunability of its active component cobalt (Co). However, there are relatively few studies on the degradation of formaldehyde in water by LaCoO₃, and the mechanism of its catalytic activity and reaction pathway are not yet fully understood.

Based on the above background, in this study, chalcogenide LaCoO₃ catalysts with different lanthanum to cobalt molar ratios were prepared by the sol-gel method, and the catalytic degradation of formaldehyde in water was systematically investigated at room temperature, and the catalytic mechanism was also revealed by the combination of the material characterization technique and the free radical burst experiments. The results of catalytic performance tests showed that the prepared LaCoO₃ catalysts exhibited excellent formaldehyde degradation activity. Compared with the traditional non-homogeneous catalysts (e.g., transition metal oxides, noble metal-loaded catalysts, etc.), the formaldehyde degradation time was shortened from 119 min to 10 min, and the degradation efficiency was improved by 12 times. The best degradation activity was achieved when the lanthanum to cobalt molar ratio was 1:1, and the complete removal of formaldehyde from water could be realized in 10 min at room temperature, and the degradation rate remained above 95% after 3 times of reuse, which showed good stability.

In order to elucidate the intrinsic reasons for the differences in catalytic activity, the surface electronic states of the catalysts with different lanthanum-cobalt molar ratios were analyzed in this study using X-ray photoelectron spectroscopy (XPS). The results showed that the relative content of Co²⁺ on the catalyst surface gradually decreased with the increase of lanthanum-cobalt molar ratio, while the content of Co³⁺ increased accordingly. Combined with the catalytic performance data, it can be found that the formaldehyde degradation activity of the catalyst is positively correlated with the Co²⁺ content, indicating that Co²⁺ is the key active site to promote the oxidative degradation of formaldehyde, and participates in the redox reaction through the Co²⁺/Co³⁺ valence cycle. reaction, accelerating the generation of active species.

In order to identify the main active species during the reaction process, this study further conducted free radical bursting experiments by adding sulfate radical (SO₄・-) bursting agent (anhydrous ethanol) and hydroxyl radical (・OH) bursting agent (tert-butanol) to the reaction system, respectively. The experimental results showed that the addition of both bursting agents significantly inhibited the degradation efficiency of formaldehyde, in which the degradation rate decreased by 681 TP3T with the addition of anhydrous ethanol and 521 TP3T with the addition of tert-butanol, which confirms that SO₄・- and ・OH are the main active species in the degradation of formaldehyde. Based on the above results, the present study proposed that the reaction mechanism of LaCoO₃-catalyzed formaldehyde degradation is a non-homogeneous Fenton-like oxidation reaction: Co²⁺ on the catalyst surface reacts with oxidants in the system (e.g., dissolved oxygen, hydrogen peroxide, etc.) to form SO₄・- and・OH, which then oxidizes formaldehyde into CO₄ and・OH through strong oxidative action. Formaldehyde is oxidized and decomposed into CO₂ and H₂O.

In this study, the potential application of chalcogenide LaCoO₃ in formaldehyde degradation in water was confirmed for the first time, the mechanism of lanthanide-cobalt molar ratio on the catalytic activity was clarified, and the reaction pathway of non-homogeneous Fenton-like oxidation was revealed, which provided the theoretical basis and technical reference for the development of highly efficient and stable catalysts for formaldehyde degradation at room temperature.

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