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计算商业ZSM-5沸石催化剂中的酸性位点

Counting the Acid Sites in a Commercial ZSM-5 Zeolite Catalyst.

作者信息

Zachariou Andrea, Hawkins Alexander P, Howe Russell F, Skakle Janet M S, Barrow Nathan, Collier Paul, Nye Daniel W, Smith Ronald I, Stenning Gavin B G, Parker Stewart F, Lennon David

机构信息

School of Chemistry, University of Glasgow, Joseph Black Building, GlasgowG12 8QQ, U.K.

UK Catalysis Hub, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, ChiltonOX11 0FA, Oxon, U.K.

出版信息

ACS Phys Chem Au. 2022 Nov 1;3(1):74-83. doi: 10.1021/acsphyschemau.2c00040. eCollection 2023 Jan 25.

DOI:10.1021/acsphyschemau.2c00040
PMID:36718264
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9881239/
Abstract

This work investigates the acid sites in a commercial ZSM-5 zeolite catalyst by a combination of spectroscopic and physical methods. The Brønsted acid sites in such catalysts are associated with the aluminum substituted into the zeolite lattice, which may not be identical to the total aluminum content of the zeolite. Inelastic neutron scattering spectroscopy (INS) directly quantifies the concentrations of Brønsted acid protons, silanol groups, and hydroxyl groups associated with extra-framework aluminum species. The INS measurements show that ∼50% of the total aluminum content of this particular zeolite is extra framework, a conclusion supported by solid-state NMR and ammonia temperature-programmed desorption (TPD) measurements. Evidence for the presence of extra-framework aluminum oxide species is also seen in neutron powder diffraction data from proton- and deuterium-exchanged samples. The differences between results from the different analytical methods are discussed, and the novelty of direct proton counting by INS in this typical commercial catalyst is emphasized.

摘要

本工作通过光谱学和物理方法相结合的方式研究了一种商用ZSM-5沸石催化剂中的酸性位点。此类催化剂中的布朗斯台德酸性位点与取代进入沸石晶格的铝相关联，这可能与沸石的总铝含量并不相同。非弹性中子散射光谱（INS）直接定量了与骨架外铝物种相关的布朗斯台德酸质子、硅醇基团和羟基的浓度。INS测量结果表明，这种特定沸石的总铝含量中约50%是骨架外的，这一结论得到了固态核磁共振和氨程序升温脱附（TPD）测量的支持。在质子和氘交换样品的中子粉末衍射数据中也发现了骨架外氧化铝物种存在的证据。讨论了不同分析方法结果之间的差异，并强调了INS在这种典型商用催化剂中直接进行质子计数的新颖性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/92876315e70b/pg2c00040_0011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/16d3bbb251ed/pg2c00040_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/85e585dcadc2/pg2c00040_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/f46f76d1c9fe/pg2c00040_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/25143b2e4d13/pg2c00040_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/4bef02ea6e1d/pg2c00040_0008.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9550/9881239/92876315e70b/pg2c00040_0011.jpg

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