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酸度在块状和纳米片状[T]MFI（T = 铝、镓、铁、硼）沸石甲醇制烃反应中的作用

On the Role of Acidity in Bulk and Nanosheet [T]MFI (T=Al Ga, Fe, B) Zeolites in the Methanol-to-Hydrocarbons Reaction.

作者信息

Meng Lingqian, Zhu Xiaochun, Mezari Brahim, Pestman Robert, Wannapakdee Wannaruedee, Hensen Emiel J M

机构信息

Inorganic Materials Chemistry, Schuit Institute of Catalysis Department of Chemical Engineering and Chemistry Eindhoven University of Technology 5600 MB Eindhoven The Netherlands.

Current address: State Key Laboratory of Heavy Oil Processing The Key Laboratory of Catalysis of CNPC College of Chemical Engineering China University of Petroleum Beijing 102249 P. R. China.

出版信息

ChemCatChem. 2017 Oct 23;9(20):3942-3954. doi: 10.1002/cctc.201700916. Epub 2017 Sep 14.

DOI:10.1002/cctc.201700916
PMID:29201243
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5698753/
Abstract

The influence of framework substituents (Al, Ga, Fe and B) and morphology (bulk vs. nanometer-sized sheets) of MFI zeolites on the acidity and catalytic performance in the methanol-to-hydrocarbons (MTH) reaction was investigated. The Brønsted acid density and strength decreased in the order Al(OH)Si>Ga(OH)Si>Fe(OH)Si≫B(OH)Si. Pyridine N NMR spectra confirmed the differences in the Brønsted and Lewis acid strengths but also provided evidence for site heterogeneity in the Brønsted acid sites. Owing to the lower efficiency with which tervalent ions can be inserted into the zeolite framework, sheet-like zeolites exhibited lower acidity than bulk zeolites. The sheet-like Al-containing MFI zeolite exhibited the greatest longevity as a MTH catalyst, outperforming its bulk [Al]MFI counterpart. Although the lower acidity of bulk [Ga]MFI led to a better catalytic performance than bulk [Al]MFI, the sheet-like [Ga]MFI sample was found to be nearly inactive owing to lower and heterogeneous Brønsted acidity. All Fe- and B-substituted zeolite samples displayed very low catalytic performance owing to their weak acidity. Based on the product distribution, the MTH reaction was found to be dominated by the olefins-based catalytic cycle. The small contribution of the aromatics-based catalytic cycle was larger for bulk zeolite than for sheet-like zeolite, indicating that shorter residence time of aromatics can explain the lower tendency toward coking and enhanced catalyst longevity.

摘要

研究了MFI沸石的骨架取代基（Al、Ga、Fe和B）以及形貌（块状与纳米尺寸薄片）对甲醇制烃（MTH）反应中酸度和催化性能的影响。布朗斯台德酸密度和强度按Al(OH)Si>Ga(OH)Si>Fe(OH)Si≫B(OH)Si的顺序降低。吡啶N NMR光谱证实了布朗斯台德酸和路易斯酸强度的差异，但也为布朗斯台德酸位点的位点不均匀性提供了证据。由于三价离子插入沸石骨架的效率较低，片状沸石的酸度低于块状沸石。片状含铝MFI沸石作为MTH催化剂表现出最长的寿命，优于其块状[Al]MFI对应物。尽管块状[Ga]MFI的较低酸度导致其催化性能优于块状[Al]MFI，但发现片状[Ga]MFI样品由于较低且不均匀的布朗斯台德酸度而几乎没有活性。所有Fe和B取代的沸石样品由于其弱酸度而表现出非常低的催化性能。基于产物分布，发现MTH反应以烯烃基催化循环为主。块状沸石中基于芳烃的催化循环的小贡献比片状沸石更大，这表明芳烃的较短停留时间可以解释较低的结焦倾向和提高的催化剂寿命。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/3c87c7ba89dc/CCTC-9-3942-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/a198b7a16e92/CCTC-9-3942-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/3ce32b7ec0eb/CCTC-9-3942-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/b76be5ca82dc/CCTC-9-3942-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/dbaa4dbdec7b/CCTC-9-3942-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/1fb6cbcedd98/CCTC-9-3942-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/7a681d67feae/CCTC-9-3942-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/938ed0876a21/CCTC-9-3942-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/5823caf1f3bb/CCTC-9-3942-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/3c87c7ba89dc/CCTC-9-3942-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/a198b7a16e92/CCTC-9-3942-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/3ce32b7ec0eb/CCTC-9-3942-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/b76be5ca82dc/CCTC-9-3942-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/dbaa4dbdec7b/CCTC-9-3942-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/1fb6cbcedd98/CCTC-9-3942-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/7a681d67feae/CCTC-9-3942-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/938ed0876a21/CCTC-9-3942-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/5823caf1f3bb/CCTC-9-3942-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3823/5698753/3c87c7ba89dc/CCTC-9-3942-g009.jpg

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