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用于间甲酚加氢脱氧制甲苯的SBA-15负载型镍铜催化剂

SBA-15 Supported Ni-Cu Catalysts for Hydrodeoxygenation of m-cresol to Toluene.

作者信息

Deplazes Roger, Teles Camila Abreu, Ciotonea Carmen, Simon Pardis, El Rassi Elias, Dhainaut Jérémy, Marinova Maya, Canilho Nadia, Richard Frédéric, Royer Sébastien

机构信息

CNRS, Centrale Lille, UMR 8181 - UCCS - Unité de Catalyse et Chimie du Solide, Univ. Artois, Université de Lille, 59000, Lille, France.

UMR 7285, Université de Poitiers, Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), rue Michel Brunet, BP633, 86022, Poitiers, France.

出版信息

ChemSusChem. 2025 Jan 2;18(1):e202400685. doi: 10.1002/cssc.202400685. Epub 2024 Sep 17.

DOI:10.1002/cssc.202400685
PMID:39004606
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11696214/
Abstract

Amidst concerns over fossil fuel dependency and environmental sustainability, the utilization of biomass-derived aromatic compounds emerges as a viable solution across diverse industries. In this scheme, the conversion of biomass involves pyrolysis, followed by a hydrodeoxygenation (HDO) step to reduce the oxygen content of pyrolysis oils and stabilize the end products including aromatics. In this study, we explored the properties of size controlled NiCu bimetallic catalysts supported on ordered mesoporous silica (SBA-15) for the catalytic gas-phase HDO of m-cresol, a lignin model compound. We compared their performances with monometallic Ni and Cu catalysts. The prepared catalysts contained varying Ni to Cu ratios and featured an average particle size of approximately 2 nm. The catalytic tests revealed that the introduction of Cu alongside Ni enhanced the selectivity for the direct deoxygenation (DDO) pathway, yielding toluene as the primary product. Optimal performance was observed with a catalyst composition comprising 5 wt.% Ni and 5 wr.% Cu, achieving 85 % selectivity to toluene. Further increasing the Cu content improved turnover frequency (TOF) values, but reduced DDO selectivity. These findings underscore the importance of catalyst design in facilitating biomass-derived compound transformations and offer insights into optimizing catalyst composition for more selective HDO reactions.

摘要

在对化石燃料依赖和环境可持续性的担忧中,生物质衍生的芳香族化合物的利用成为跨行业可行的解决方案。在此方案中,生物质的转化包括热解,随后是加氢脱氧(HDO)步骤,以降低热解油的氧含量并稳定包括芳烃在内的最终产物。在本研究中,我们探索了负载在有序介孔二氧化硅(SBA-15)上的尺寸可控的镍铜双金属催化剂对木质素模型化合物间甲酚的催化气相HDO性能。我们将它们的性能与单金属镍和铜催化剂进行了比较。制备的催化剂含有不同的镍铜比,平均粒径约为2 nm。催化试验表明,与镍一起引入铜提高了直接脱氧(DDO)途径的选择性,甲苯是主要产物。在含有5 wt.%镍和5 wt.%铜的催化剂组合物中观察到最佳性能,对甲苯的选择性达到85%。进一步增加铜含量提高了周转频率(TOF)值,但降低了DDO选择性。这些发现强调了催化剂设计在促进生物质衍生化合物转化中的重要性,并为优化催化剂组成以实现更具选择性的HDO反应提供了见解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/fe742494e88a/CSSC-18-e202400685-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/f46966b0ccd2/CSSC-18-e202400685-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/db27de94bdb6/CSSC-18-e202400685-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/ef5ab07aebe8/CSSC-18-e202400685-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/e50e2ad70a2b/CSSC-18-e202400685-g015.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/4e5de2e82251/CSSC-18-e202400685-g013.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/81084ba6c9b9/CSSC-18-e202400685-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/d7c5478dfe81/CSSC-18-e202400685-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/fe742494e88a/CSSC-18-e202400685-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/f46966b0ccd2/CSSC-18-e202400685-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/db27de94bdb6/CSSC-18-e202400685-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/ef5ab07aebe8/CSSC-18-e202400685-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/e50e2ad70a2b/CSSC-18-e202400685-g015.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/4e5de2e82251/CSSC-18-e202400685-g013.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/81084ba6c9b9/CSSC-18-e202400685-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/d7c5478dfe81/CSSC-18-e202400685-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3863/11696214/fe742494e88a/CSSC-18-e202400685-g005.jpg

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