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金红石相锡钛混合氧化物作为水相中碳-碳含氧化合物缩合反应的酸催化剂。

Rutile-Phase Sn-Ti Mixed Oxides as Acid Catalysts for the Condensation of C-C Oxygenated Compounds in Water.

作者信息

Fernández-Arroyo A, Domine Marcelo E

机构信息

Instituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València., Consejo Superior de Investigaciones Científicas., Avda. Los Naranjos s/n 46022, Valencia, Spain.

出版信息

ChemSusChem. 2025 Apr 14;18(8):e202401761. doi: 10.1002/cssc.202401761. Epub 2024 Nov 12.

DOI:10.1002/cssc.202401761
PMID:39401171
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11997911/
Abstract

The design of new cost-effective and water-resistant acid catalysts is crucial for valorizing aqueous side-streams to increase the efficiency and competitiveness of bio-refineries in a sustainable way. In this work, Sn-Ti mixed oxides are prepared via a green and scalable co-precipitation method. This synthesis procedure allows obtaining homogeneous rutile-phase Sn-Ti mixed oxides with enhanced textural properties and a higher amount of Lewis acid sites. More importantly, the catalytic behavior of these Sn-Ti mixed oxides is investigated by using an aqueous mixture of C-C representative oxygenated compounds, closer to real industrial conditions and differing from usual individual probe molecules studies performed even in the absence of water. Catalytic experiments combined and correlated with spectroscopic measurements (i. e., XRD, TEM, FT-IR with pyridine adsorption-desorption and N adsorption) are performed to better understand the properties of different Sn-Ti catalysts. These materials show promising results in the condensation of light oxygenated compounds present in aqueous fractions. Homogeneous and robust rutile-phase structures with inherent hydrophobic characteristics turn these Sn-Ti materials into active and highly resistant catalysts capable to transform these low-value oxygenated compounds into a mixture of hydrocarbons and aromatics useful for blending with automotive fuels, especially under complex acidic aqueous environments and moderate process conditions.

摘要

设计新型经济高效且防水的酸催化剂对于将含水副产物转化为高附加值产品至关重要,这能够以可持续的方式提高生物炼制厂的效率和竞争力。在这项工作中,通过绿色且可扩展的共沉淀法制备了Sn-Ti混合氧化物。该合成过程能够获得具有增强的织构性质和更高数量路易斯酸位点的均匀金红石相Sn-Ti混合氧化物。更重要的是,使用C-C代表性含氧化合物的水性混合物研究了这些Sn-Ti混合氧化物的催化行为,该混合物更接近实际工业条件,与通常即使在无水情况下进行的单个探针分子研究不同。结合催化实验并与光谱测量(即XRD、TEM、吡啶吸附-脱附的FT-IR和N吸附)相关联,以更好地了解不同Sn-Ti催化剂的性质。这些材料在含水馏分中存在的轻质含氧化合物的缩合反应中显示出有前景的结果。具有固有疏水特性的均匀且坚固的金红石相结构使这些Sn-Ti材料成为活性且高度耐用的催化剂,能够将这些低价值含氧化合物转化为可用于与汽车燃料混合的烃类和芳烃混合物,特别是在复杂的酸性水性环境和适度的工艺条件下。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/e7e1c7fe198d/CSSC-18-e202401761-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/8901f61e4d4e/CSSC-18-e202401761-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/5ee4f2386fbd/CSSC-18-e202401761-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/d16905d59454/CSSC-18-e202401761-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/e7e1c7fe198d/CSSC-18-e202401761-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/8901f61e4d4e/CSSC-18-e202401761-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/5ee4f2386fbd/CSSC-18-e202401761-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/d16905d59454/CSSC-18-e202401761-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bc5/11997911/e7e1c7fe198d/CSSC-18-e202401761-g005.jpg

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