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Environmentally benign melamine functionalized silica-coated iron oxide for selective CO2 capture and fixation into cyclic carbonate
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-05-15 , DOI: 10.1016/j.jcou.2021.101575
Nikita Guha , Anoop K. Gupta , Sobhan Chatterjee , Sarathkumar Krishnan , Mayank K. Singh , Dhirendra K. Rai

The development of new materials capable of fixing CO2 into value-added products has become an exciting research field. Besides mitigating the rising level of CO2, such materials also enable CO2 as a C1 carbon source for useful industrial synthons. This article reports on the stepwise synthesis of a melamine functionalized silica-coated iron oxide (FSNM) material for selective CO2 capture and its catalytic conversion into a useful product. The synthesis of FSNM has been achieved by covalently grafting the melamine group in the pores of mesoporous silica-coated Fe3O4 (Fe3O4@SiO2) particle using isocyanate as a cross-linker. While the Fe3O4 core, owing to its superparamagnetic property, enables the easy retrieval of the material from the reaction mixture and, thus, enhances the recyclability, mesoporous silica coating offers a larger surface area for adsorption. The organic functionalities, containing melamine and carbamide moieties, facilitate the selective adsorption of CO2 on the material with a maximum CO2 uptake of 0.48 mmol/g at 1 bar and 298 K with excellent CO2/N2 selectivity. Moreover, the acid-base interactions between the acidic CO2 and basic amine groups enable the FSNM to catalyze the cycloaddition of CO2 with different epoxides to afford a series of cyclic carbonates, in the presence of tetrabutylammonium bromide (TBAB) as a co-catalyst, under facile and solvent-free conditions. These results strongly support that melamine functionalized Fe3O4@SiO2 affords new aspects towards environmentally friendly and recoverable hybrid adsorbent for adsorption and fixation of CO2 into the valuable products.



中文翻译:

环境友好的三聚氰胺官能化二氧化硅包覆的氧化铁,用于选择性捕获CO 2并将其固定在环状碳酸酯中

能够将CO 2固定在增值产品中的新材料的开发已经成为令人兴奋的研究领域。除了减轻CO 2的上升水平外,此类材料还使CO 2成为有用的工业合成器的C1碳源。本文报道了逐步合成三聚氰胺功能化的二氧化硅涂层的氧化铁(FSNM)材料,用于选择性捕获CO 2及其催化转化为有用的产品。FSNM的合成是通过将三聚氰胺基团共价接枝到介孔二氧化硅包覆的Fe 3 O 4(Fe 3 O 4 @SiO)的孔中而实现的2)使用异氰酸酯作为交联剂的颗粒。Fe 3 O 4核由于具有超顺磁性,因此可以轻松地从反应混合物中回收材料,从而提高了可回收性,而介孔二氧化硅涂层则提供了更大的吸附表面积。包含三聚氰胺和尿素基团的有机官能团有助于在材料上以1 bar的最大CO 2吸收量为0.48 mmol / g和298 K的情况下选择性吸附CO 2,并且具有出色的CO 2 / N 2选择性。此外,酸性CO 2和碱性胺基之间的酸碱相互作用使FSNM成为可能在四丁基溴化铵(TBAB)作为助催化剂的条件下,在方便且无溶剂的条件下,用不同的环氧化物催化CO 2的环加成反应,得到一系列环状碳酸酯。这些结果有力地证明了三聚氰胺官能化的Fe 3 O 4 @SiO 2为环保和可回收的混合吸附剂提供了新的方面,以将CO 2吸附和固定在有价值的产品中。

更新日期:2021-05-15
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