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Comprehensive understanding of base catalysis derived from nitrogen species incorporated into the frameworks of silica and carbon porous materials
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2024-02-24 , DOI: 10.1016/j.micromeso.2024.113070
Aisa Kawano , Ayumi Sato , Yuki Nakamura , Akira Nakayama , Takahiko Moteki , Masaru Ogura

A base-catalytic nitrogen site in a specific and confined nanospace on the surfaces of silica and carbon was developed using mesoporous silica SBA-15 and its replicated porous carbon nitride PCN. Knoevenagel condensation reactions using differentially active methylene compounds and diffusion studies using CO as the probe molecule for the basic site revealed that the primary amine-based N component showed high activity for the base-catalyzed reaction. Among the samples investigated, primary amine-grafted SBA-15 showed the highest performance owing to the activity and location density of primary amines, as well as its surrounding hydrophobic nature. Although NSBA-15 showed moderate catalytic performance owing to an isolated active N species located on its mesopore surface, methylation of the N species led to enhanced catalytic performance because of its isolation effect. Carbonaceous PCN showed high hydrophobicity and durability during reaction and storage. A general design for N-based basic catalytic materials was also proposed.

中文翻译:

全面了解二氧化硅和碳多孔材料骨架中氮物质的碱催化作用

使用介孔二氧化硅 SBA-15 及其复制的多孔氮化碳 PCN 开发了二氧化硅和碳表面特定且受限的纳米空间中的碱催化氮位点。使用不同活性亚甲基化合物的 Knoevenagel 缩合反应和使用 CO 作为碱性位点探针分子的扩散研究表明,伯胺基 N 组分对碱催化反应表现出高活性。在所研究的样品中,由于伯胺的活性和位置密度及其周围的疏水性,伯胺接枝的 SBA-15 显示出最高的性能。尽管 NSBA-15 由于其介孔表面上存在孤立的活性 N 物种而表现出中等催化性能,但 N 物种的甲基化由于其隔离效应而导致催化性能增强。碳质PCN在反应和储存过程中表现出高疏水性和耐久性。还提出了氮基基础催化材料的总体设计。
更新日期:2024-02-24
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