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作为铜活性位点载体的分级SAPO-34催化剂。

Hierarchical SAPO-34 Catalysts as Host for Cu Active Sites.

作者信息

Fernandes Pape Brito Julio C, Miletto Ivana, Marchese Leonardo, Ali Daniel, Azim Muhammad Mohsin, Mathisen Karina, Gianotti Enrica

机构信息

Department for Sustainable Development and Ecological Transition, Università del Piemonte Orientale, Piazza Sant'Eusebio 5, 13100 Vercelli, Italy.

Department of Pharmaceutical Sciences, Università del Piemonte Orientale, Largo Donegani 2, 28100 Novara, Italy.

出版信息

Materials (Basel). 2023 Aug 19;16(16):5694. doi: 10.3390/ma16165694.

DOI:10.3390/ma16165694
PMID:37629985
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10456513/
Abstract

Cu-containing hierarchical SAPO-34 catalysts were synthesized by the bottom-up method using different mesoporogen templates: CTAB encapsulated within ordered mesoporous silica nanoparticles (MSNs) and sucrose. A high fraction of the Cu centers exchanged in the hierarchical SAPO-34 architecture with high mesopore surface area and volume was achieved when CTAB was embedded within ordered mesoporous silica nanoparticles. Physicochemical characterization was performed by using structural and spectroscopic techniques to elucidate the properties of hierarchical SAPO-34 before and after Cu introduction. The speciation of the Cu sites, investigated by DR UV-Vis, and the results of the catalytic tests indicated that the synergy between the textural properties of the hierarchical SAPO-34 framework, the high Cu loading, and the coordination and localization of the Cu sites in the hierarchical architecture is the key point to obtaining good preliminary results in the NO selective catalytic reduction with hydrocarbons (HC-SCR).

摘要

采用自下而上的方法,使用不同的介孔生成模板:封装在有序介孔二氧化硅纳米颗粒(MSN)中的十六烷基三甲基溴化铵(CTAB)和蔗糖,合成了含铜的分级SAPO-34催化剂。当CTAB嵌入有序介孔二氧化硅纳米颗粒中时,在具有高介孔表面积和体积的分级SAPO-34结构中实现了高比例的铜中心交换。通过结构和光谱技术进行物理化学表征,以阐明引入铜之前和之后分级SAPO-34的性质。通过漫反射紫外可见光谱(DR UV-Vis)研究的铜位点的形态以及催化测试结果表明,分级SAPO-34骨架的织构性质、高铜负载量以及铜位点在分级结构中的配位和定位之间的协同作用是在烃类选择性催化还原NO(HC-SCR)中获得良好初步结果的关键。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/ac1c7c76a1b9/materials-16-05694-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/d9437e7be959/materials-16-05694-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/97e7fd9cc71e/materials-16-05694-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/dac8012237c2/materials-16-05694-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/4d23aac78610/materials-16-05694-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/ac1c7c76a1b9/materials-16-05694-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/d9437e7be959/materials-16-05694-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/97e7fd9cc71e/materials-16-05694-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/dac8012237c2/materials-16-05694-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/4d23aac78610/materials-16-05694-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/faa7/10456513/ac1c7c76a1b9/materials-16-05694-g005.jpg

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本文引用的文献

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Stabilizing the framework of SAPO-34 zeolite toward long-term methanol-to-olefins conversion.稳定SAPO-34沸石框架以实现长期甲醇制烯烃转化
Nat Commun. 2021 Aug 2;12(1):4661. doi: 10.1038/s41467-021-24403-2.
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Improved lifetime and stability of copper species in hierarchical, copper-incorporated CuSAPO-34 verified by catalytic model reactions.
通过催化模型反应验证了分级结构且含铜的CuSAPO-34中铜物种的寿命和稳定性得到了提高。
Phys Chem Chem Phys. 2021 Aug 12;23(31):16785-16794. doi: 10.1039/d1cp01898a.
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Characterization of Nanoporous Materials.纳米多孔材料的表征
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State of the Art and Perspectives of Hierarchical Zeolites: Practical Overview of Synthesis Methods and Use in Catalysis.分级沸石的现状与展望:合成方法及催化应用的实践概述
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