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Silica extracts from fly ash modified via sol-gel methods and functionalized with CMPO for potential scavenging of rare earth elements La³⁺ and Ce³⁺
Materials Chemistry and Physics ( IF 4.6 ) Pub Date : 2024-04-03 , DOI: 10.1016/j.matchemphys.2024.129161
Mauricio Gómez , Jaime Pizarro , Carlos Díaz , Claudia Ortiz , Ximena Castillo , Miriam Navlani-García , Diego Cazorla-Amorós

A mesoporous material was synthesized using silica extracts from fly ash and its properties were studied. Subsequently, it was functionalized with carbamoylmethylphosphine oxide (CMPO) to capture La and Ce. The developed mesoporous material was obtained by the sol-gel method and was called Si-MMS (siliceous mesoporous materials), subsequently functionalized with APTMS (1-(2-aminoethyl)-3-aminopropyl trimethoxysilane) in a reflux system, which led to the synthesis of Si-MMS-APTMS. This derivative was modified with carbonyldiimidazole (CDI) and diethylphosphonoacetic acid, which finally resulted in the synthesis of Si-MMS-CMPO as the final product. The materials were characterized by DRIFT, XRD, SEM-EDS, TEM, XPS, elemental analysis and nitrogen isotherms at −196 °C, confirming that the synthesis and subsequent modification of the mesoporous structure was successful. Adsorption studies in batch systems indicated that the optimal pH for La was 6, the Langmuir isotherm model and the non-linear Sips models were perfectly fitted and the best fitting kinetics is the Elovich model. For Ce the optimal pH was 7.5, the non-linear Sips isotherm fit the best and the non-linear Pseudo-second order kinetics was the mechanism that best represents the adsorption. The maximum experimental adsorption capacity q of La was 17.00 mg g and for Ce was 30.09 mg g. In both cases, the rapid adsorption suggests an open porous matrix that facilitates the formation of chelates between the adsorbates and the phosphoryl group -PO.

中文翻译:

通过溶胶-凝胶法对飞灰中的二氧化硅提取物进行改性,并用 CMPO 进行功能化,以清除稀土元素 La3⁺ 和 Ce3⁺

利用飞灰中的二氧化硅提取物合成了介孔材料并研究了其性能。随后,用氨基甲酰基甲基氧化膦(CMPO)对其进行功能化以捕获 La 和 Ce。所开发的介孔材料是通过溶胶-凝胶法获得的,称为Si-MMS(硅质介孔材料),随后在回流系统中用APTMS(1-(2-氨基乙基)-3-氨基丙基三甲氧基硅烷)进行功能化,从而得到Si-MMS-APTMS的合成。该衍生物用羰基二咪唑(CDI)和二乙基膦酰乙酸进行修饰,最终合成最终产物Si-MMS-CMPO。通过DRIFT、XRD、SEM-EDS、TEM、XPS、元素分析和-196℃氮等温线对材料进行了表征,证实介孔结构的合成和后续修饰是成功的。间歇系统的吸附研究表明,La的最佳pH为6,Langmuir等温线模型和非线性Sips模型完美拟合,最佳拟合动力学是Elovich模型。对于 Ce,最佳 pH 值为 7.5,非线性 Sips 等温线拟合最佳,非线性伪二级动力学是最能代表吸附的机制。 La 的最大实验吸附容量 q 为 17.00 mg g-1,Ce 的最大实验吸附容量 q 为 30.09 mg g-1。在这两种情况下,快速吸附表明开放多孔基质有利于吸附物和磷酰基-PO 之间形成螯合物。
更新日期:2024-04-03
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