Quantifying the fraction and activity of catalytic sites at different surface densities of aminosilanes in SBA-15 for the aldol reaction and condensation
Quantifying the fraction and activity of catalytic sites at different surface densities of aminosilanes in SBA-15 for the aldol reaction and condensation
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量化 SBA-15 中氨基硅烷不同表面密度下羟醛反应和缩合催化位点的分数和活性
DOI：
10.1016/j.jcat.2022.08.015
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发表时间：
2022
影响因子：
7.3
通讯作者：
Brunelli, Nicholas A.
中科院分区：
文献类型：
--
作者：
Chen, Jee-Yee;Pineault, Hannah;Brunelli, Nicholas A.
氨基二氧化硅材料的复杂性表现为具有多种活性中心的催化剂。以前的工作假设每个地点对观察到的催化行为的贡献是相等的，而这项工作使用地点量化实验严格地研究了每个地点的催化活性。这些实验表明，氨基二氧化硅材料有四种类型的催化中心，包括高、中、低活性中心以及非活性中心。每个位置的比例取决于表面密度。低活性中心与聚集在表面的胺有关。进一步的实验表明，高活性中心可能与成对接枝的胺或位于外表面的胺无关，这使得我们推测不同的是胺与不同类型的硅烷醇协同作用。总体而言，这些结果证明了利用合作作用创造高活性催化材料的潜力。
The complexity of aminosilica materials manifests as catalysts with multiple types of active sites. Whereas previous work has assumed that each site contributes equally to the observed catalytic behavior, this work rigorously investigates the catalytic activity on a per site basis using site quantification experiments. These experiments reveal that aminosilica materials have four types of catalytic sites, including high, medium, and low activity sites as well as inactive sites. The fraction of each of these sites depends on the surface density. The low activity sites are associated with amines clustered on the surface. Additional experiments reveal that the high activity sites are likely not associated with amines grafted in pairs or amines located on the external surface, leading us to speculate that the difference is amines cooperatively interacting with different types of silanols. Overall, the results demonstrate the potential to create highly active catalytic materials using cooperative interactions.
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影响因子：
9.9
作者：
F. Shang;Jianrui Sun;Shujie Wu;Hengli Liu;J. Guan;Q. Kan
通讯作者：
F. Shang;Jianrui Sun;Shujie Wu;Hengli Liu;J. Guan;Q. Kan
影响因子：
15
作者：
Hoang, L;Bahmanyar, S;List, B
通讯作者：
List, B
影响因子：
12.9
作者：
Ellebracht, Nathan C.;Jones, Christopher W.
通讯作者：
Jones, Christopher W.
羟醛反应的过渡结构
影响因子：
15
作者：
Yi Li;M. Paddon;K. Houk
通讯作者：
K. Houk
影响因子：
10.7
作者：
Tafida UI;Uzairu A;Abechi SE
通讯作者：
Abechi SE