支撑酸度对β-SBA-16和Al-SBA-16底物上HDS性能的影响：组合的实验和理论研究,Energy & Fuels

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支撑酸度对β-SBA-16和Al-SBA-16底物上HDS性能的影响：组合的实验和理论研究
Energy & Fuels ( IF 5.2 ) Pub Date : 2019-01-23 00:00:00 , DOI: 10.1021/acs.energyfuels.8b04133
Peng Zheng ₁ , Di Hu ₁ , Qian Meng ₁ , Cong Liu ₁ , Xilong Wang ₁ , Jiyuan Fan ₁ , Aijun Duan ₁ , Chunming Xu ₁

Affiliation

成功合成了新型复合材料β-SBA-16，并用作开发加氢脱硫（HDS）催化剂的载体。通过包括X射线衍射，N ₂物理吸附，²⁷ Al NMR，拉曼，吡啶IR，X射线光电子能谱和高分辨率透射电子显微镜的各种技术来表征载体和相应的催化剂。活性评估结果表明，与负载在Al改性SBA-16和常规催化剂上的催化剂相比，NiMo /β-SBA-16催化剂在20 h ^–1的重时空速下具有最高的97.3％的二苯并噻吩HDS效率。铝₂ O ₃。此外，NiMo /β-SBA-16在150 h ^–1时的HDS效率几乎是其他两种催化剂的1.5倍。，这被认为与载体的酸性密切相关。相应地，吡啶IR的结果表明NiMo /β-SBA-16具有较大的总酸度和较高的B / L酸度比。此外，进行了密度泛函理论计算，以探索由于掺入β晶种或Al原子而产生的布朗斯台德酸强度。计算结果表明，位于β沸石5或6元环上的Si原子更容易被Al原子取代，并且生成的Si-OH-Al基团在提供更强的Brønsted酸位方面起着重要作用。因此，实验和理论结果均表明，掺入β种子有助于产生SBA-16材料的布朗斯台德酸位。

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Influence of Support Acidity on the HDS Performance over β-SBA-16 and Al-SBA-16 Substrates: A Combined Experimental and Theoretical Study

A novel composite material β-SBA-16 is successfully synthesized and utilized as the support for the development of hydrodesulfurization (HDS) catalyst. The supports and the corresponding catalysts were characterized by a variety of techniques involving X-ray diffraction, N₂ physisorption, ²⁷Al NMR, Raman, pyridine IR, X-ray photoelectron spectra, and high-resolution transmission electron microscopy. The activity evaluation results displayed that the NiMo/β-SBA-16 catalyst possessed the highest dibenzothiophene HDS efficiency of 97.3% at weight hourly space velocity of 20 h^–1 compared with the catalysts supported on the Al-modified SBA-16 and the conventional Al₂O₃. Furthermore, the HDS efficiency of NiMo/β-SBA-16 is almost 1.5 times that of the other two catalysts at 150 h^–1, which was considered to be closely linked to the acidic properties of the supports. Correspondingly, the results of pyridine IR exhibited that NiMo/β-SBA-16 possessed larger amounts of total acidity and higher B/L acidities ratio. Furthermore, density functional theory calculations were performed to explore the Brønsted acid strength generated by the incorporation of β seeds or Al atoms. The calculation results indicated that Si atoms located in the 5- or 6-membered rings of β-zeolite were more easily substituted by Al atoms, and the generated Si–OH–Al group played an important role in providing stronger Brønsted acid sites. Therefore, both experimental and theoretical results have shown that the incorporation of β seeds contributed more to produce the Brønsted acid sites of SBA-16 materials.

更新日期：2019-01-23

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