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Highly water-soluble dimeric and trimeric lanthanide carbonates with ethylenediaminetetraacetates as precursors of catalysts for the oxidative coupling reaction of methane
New Journal of Chemistry ( IF 3.3 ) Pub Date : 2022-01-19 , DOI: 10.1039/d1nj05608e
Rong-Yan Lin 1 , Yan-Ru Shi 1 , Yu-Hui Hou 1 , Wen-Sheng Xia 1 , Wei-Zheng Weng 1 , Zhao-Hui Zhou 1
Affiliation  

Reactions of carbon dioxide with lanthanide ethylenediaminetetraacetates M[Ln(EDTA)(H2O)3]·5H2O (M = NH4, Na or K; Ln = La or Ce) result in the formation of highly water-soluble lanthanide carbonates with ethylenediaminetetraacetates (NH4)5[La3(CO3)(EDTA)3(H2O)3]·12H2O (1), Na8[Ln2(CO3)3(EDTA)2]·17.5H2O (Ln = La, 2; Ce, 3), and K5[Ln3(CO3)(EDTA)3(H2O)3]·13.5H2O (Ln = La, 4; Ce, 5; H4EDTA = ethylenediaminetetraacetic acid) in dimethylformamide–water solution, which have been fully characterized. The main structures of these five complexes are all based on the [Ln(EDTA)] unit, where carbonates participate due to coordination in μ12(O,O) and μ22(O,O′):η2(O,O′) fashion. The reactions of lanthanum ethylenediaminetetraacetate with CO2 have been monitored via13C NMR measurements. Furthermore, the calcined products of 1 and 2 are used for the oxidative coupling reaction of methane (OCM). The results demonstrate the good catalytic performances of La2O3 or La2O2CO3 from 1 and a mixture of La2O2CO3 and Na2CO3 from 2. The coordination modes of the lanthanide carbonates in precursors 1 and 2 may provide a model for the interaction of lanthanide carbonates, which is useful for the OCM reaction.

中文翻译:

高水溶性二聚和三聚镧系元素碳酸盐与乙二胺四乙酸盐作为甲烷氧化偶联反应催化剂的前体

二氧化碳与镧系元素乙二胺四乙酸盐 M[Ln(EDTA)(H 2 O) 3 ]·5H 2 O(M = NH 4、Na 或 K;Ln = La 或 Ce)反应生成高度水溶性的镧系元素碳酸盐与乙二胺四乙酸盐 (NH 4 ) 5 [La 3 (CO 3 )(EDTA) 3 (H 2 O) 3 ]·12H 2 O ( 1 ), Na 8 [Ln 2 (CO 3 ) 3 (EDTA) 2 ]· 17.5H 2 O (Ln = La, 2 ; Ce,3 ), 和 K 5 [Ln 3 (CO 3 )(EDTA) 3 (H 2 O) 3 ]·13.5H 2 O (Ln = La, 4 ; Ce, 5 ; H 4 EDTA = 乙二胺四乙酸)在二甲基甲酰胺中–水溶液,已充分表征。这五种配合物的主要结构均基于[Ln(EDTA)] -单元,其中碳酸盐由于在μ 12 (O,O) 和μ 22 (O,O')中的配位而参与其中:η 2(O,O') 时尚。已通过13 C NMR 测量监测乙二胺四乙酸镧与 CO 2的反应。此外,12的煅烧产物用于甲烷的氧化偶联反应(OCM)。结果表明来自1的La 2 O 3La 2 O 2 CO 3以及来自2的La 2 O 2 CO 3和Na 2 CO 3的混合物具有良好的催化性能。. 前驱体12中镧系元素碳酸盐的配位模式可以为镧系元素碳酸盐的相互作用提供模型,这对 OCM 反应很有用。
更新日期:2022-01-19
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