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具有三维介孔结构的钒掺杂介孔二氧化硅用于丙烯环氧化的设计、合成及催化性能

The design, synthesis and catalytic performance of vanadium-incorporated mesoporous silica with 3D mesoporous structure for propene epoxidation.

作者信息

Held Agnieszka, Janiszewska Ewa, Czerepińska Justyna, Kowalska-Kuś Jolanta

机构信息

Adam Mickiewicz University, Faculty of Chemistry Uniwersytetu Poznańskiego 8 61614 Poznan Poland

出版信息

RSC Adv. 2020 Mar 10;10(17):10144-10154. doi: 10.1039/d0ra00349b. eCollection 2020 Mar 6.

Abstract

V-containing mesoporous silica with 3D structure was prepared by a hydrothermal procedure using NHVO as the vanadium precursor and with varied reaction mixture pH values (pH = 3 and pH = 5). The combined use of DR UV-vis and H-TPR techniques confirmed the successful incorporation of vanadium into the structure of the mesoporous silica material. The number of acid sites, evidenced by ammonia TPD, strongly correlates with the vanadium content. Propene oxidation with NO revealed the noticeable activity of the synthesised vanadium-containing mesoporous materials in epoxidation reactions. The activity of the synthesized vanadosilicates is compared with the performance of vanadium-supported catalysts (on mesoporous silica of 3D structures) prepared by wet-impregnation method. On the basis of TOF analysis indicating the activity of particular vanadium ions, it was evidenced that although the presence of isolated V species is crucial in propene epoxidation, the availability of the active species is of paramount importance for proper vanadium utilization.

摘要

以NHVO为钒前驱体,通过水热法在不同反应混合物pH值(pH = 3和pH = 5)下制备了具有三维结构的含钒介孔二氧化硅。DR紫外可见光谱和H-TPR技术的联合使用证实了钒成功掺入介孔二氧化硅材料的结构中。氨程序升温脱附证明的酸位数量与钒含量密切相关。丙烯与NO的氧化反应表明合成的含钒介孔材料在环氧化反应中具有显著活性。将合成的钒硅酸盐的活性与通过湿浸渍法制备的负载型钒催化剂(在三维结构的介孔二氧化硅上)的性能进行了比较。基于表明特定钒离子活性的TOF分析,证明尽管孤立的V物种的存在对丙烯环氧化至关重要,但活性物种的可用性对于钒的合理利用至关重要。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5528/9050468/1ebf8dc70dfa/d0ra00349b-f1.jpg

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