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Particularities of trichloroethylene photocatalytic degradation over crystalline RbLaTa2O7 nanowire bundles grown by solid-state synthesis route

DOI:10.1016/j.jece.2018.11.034 期刊:Journal of Environmental Chemical Engineering 出版年份:2018 更新时间:2025-09-23 15:21:21
摘要: This is the first report on synthesis and photocatalytic activity for trichloroethylene (TCE) degradation under simulated solar light over RbLaTa2O7 layered perovskites with predominant nanowire or platelet morphologies. SEM images witnessed that the one step thermal treatment at 1200 °C lead to formation of RbLaTa2O7 nanowires with diameter of 80~320 nm and several microns in length associated in bundles and sharp-edged, merged platelets (minor phase). The two-step annealing at 950 °C and 1200 °C resulted in decrease of wires bundle population and increase in that of platelets merged in facetted particles. The RbLaTa2O7 nanowires are made of by well-aligned atomic rows with preferred orientation toward the c-axis, relatively free of defect. High density of hydroxyl groups on the sample calcined in mild conditions (RbLaTa_01) favors the photo mineralization of TCE. In contrast, the activity of RbLaTa_02 annealed in harsh conditions (950 and 1200 oC), poor in surface hydroxyl groups, remained modest. The weak surface basicity directed the reaction mainly to generation of intermediate chlorinated compounds. Pd and Au were supported on RbLaTa2O7 perovskites as an alternative strategy to boost the removal of chlorinated pollutants by combining photocatalytic (mineralization) and catalytic (hydrodechlorination, HDC) processes. The mineralization of TCE to Cl- was drastically hindered in presence of methanol due to quenching of ?OH radicals by alcohol. The results suggested that the density of RbLaTa2O7 surface hydroxyl groups is essential for photo mineralization of TCE whereas the surface carbonate is beneficial for the formation of intermediate chlorinated product.
作者: Monica Raciulete,Florica Papa,Daisuke Kawamoto,Cornel Munteanu,Daniela C. Culita,Catalin Negrila,Irina Atkinson,Veronica Bratan,Jeanina Pandele-Cusu,Ioan Balint
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Investigating the synthesis and photocatalytic activity of RbLaTa2O7 layered perovskites for the degradation of trichloroethylene (TCE) under simulated solar light.

The study demonstrated that the density of RbLaTa2O7 surface hydroxyl groups is essential for photo mineralization of TCE, whereas the surface carbonate is beneficial for the formation of intermediate chlorinated product. The findings suggest that milder preparation methods should be developed to enhance the photocatalytic activity.

The elevated synthesis temperature leads to a decrease in the density of surface -OH groups, which are involved in the generation of strongly oxidizing ?OH radicals. Milder preparation methods should be envisaged in the future to obtain materials with large surface areas and high density of surface -OH groups.

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