Hosting AlCl3 on ternary metal oxide composites for catalytic oligomerization of 1-decene: Revealing the role of supports via performance evaluation and DFT calculation
Hosting AlCl3 on ternary metal oxide composites for catalytic oligomerization of 1-decene: Revealing the role of supports via performance evaluation and DFT calculation
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在三元金属氧化物复合材料上承载 AlCl3 用于催化 1-癸烯齐聚：通过性能评估和 DFT 计算揭示载体的作用
DOI：
10.1016/j.micromeso.2021.111665
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发表时间：
2021-12
影响因子：
5.2
通讯作者：
Yujun Tong
中科院分区：
文献类型：
--
作者：
Yue Lou;Yuxiang Chen;Yang Zhao;Cheng Qian;Cheng Niu;Hao Jiang;Chuanlei Liu;Kongguo Wu;Benxian Shen;Jian Long;Yiming Wang;Hui Sun;Jigang Zhao;Jichang Liu;Hao Ling;Di Wu;Yujun Tong
由于对活性组分与载体之间相互作用的了解有限且调节不令人满意，增强负载型路易斯酸催化剂的催化活性和稳定性仍然是一个特殊的挑战。在此，我们将AlCl3固定在La2O3-Al2O3-SiO2、NiO-Al2O3-SiO2和Ga2O3-Al2O3-SiO2等一系列三元金属氧化物上，通过实验和密度泛函理论（DFT）计算，清楚地揭示了载体的组成和结构对催化剂性能的影响。使用间歇反应器和固定床装置通过 1-癸烯的低聚来评估负载样品的催化性能。结果表明，NiO-Al2O3-SiO2 复合材料负载的 AlCl3 由于其正孔结构和活性物质的高负载量而表现出最高的催化活性和稳定性。重要的是，DFT计算表明三元氧化物复合材料和AlCl3之间的主客体相互作用能的变化与实验结果非常吻合。这项研究强调了载体的组成和结构对路易斯酸催化剂的催化性能至关重要，并为高性能负载型催化剂的设计提供了基础指导。
Enhancing catalytic activity and stability of supported Lewis acid catalysts remain a particular challenge owing to the limited understanding and unsatisfactory tuning of the interplay between the active components and the supports. Herein, upon immobilizing AlCl3on a series of ternary metal oxides including La2O3–Al2O3–SiO2, NiO–Al2O3–SiO2and Ga2O3–Al2O3–SiO2, we clearly revealed the influence of the compositions and structures of the supports on the catalyst performances through experiments together with density functional theory (DFT) calculations. The catalytic performances of the supported samples were evaluated by oligomerization of 1-decene using both batch reactor and fixed-bed apparatus. The results suggest that the AlCl3supported by NiO–Al2O3–SiO2composites exhibits the highest catalytic activity and stability because of its positive pore structure and thereof the high loading of active species. Importantly, DFT calculations indicate that the variations of the host-guest interaction energy between the ternary oxide composites and AlCl3are in good agreement with the experimental results. This study highlights the compositions and structures of the supports are crucial to the catalytic performances of Lewis acid catalysts, and provides fundamental guidance for design of high-performance supported catalysts.
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路易斯酸催化水中吡咯的对映选择性傅克烷基化
影响因子：
4.1
作者：
Sun Jianan;Gui Yang;Huang Yekai;Li Jindong;Zha Zhenggen;Yang Yu;Wang Zhiyong
通讯作者：
Wang Zhiyong
影响因子：
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作者：
Anuj Joshi;Harmen S. Zijlstra;S. Collins;J. McIndoe
通讯作者：
Anuj Joshi;Harmen S. Zijlstra;S. Collins;J. McIndoe
DOI：
10.1021/acs.jpcc.1c00691
发表时间：
2021-01
期刊：
The Journal of Physical Chemistry C
影响因子：
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作者：
M. Radue;S. Baek;Azadeh Farzaneh;K. Dwyer;Q. Campbell;A. Baczewski;E. Bussmann;George T. Wang;Yifei Mo;S. Misra;R. Butera
通讯作者：
M. Radue;S. Baek;Azadeh Farzaneh;K. Dwyer;Q. Campbell;A. Baczewski;E. Bussmann;George T. Wang;Yifei Mo;S. Misra;R. Butera
影响因子：
3.7
作者：
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通讯作者：
Hiromasa Shiiba;N. Zettsu;M. Nakayama;S. Oishi;Katsuya Teshima
影响因子：
22.1
作者：
V. Krishna;G. Naresh;Vikas Kumar;R. Sarkari;A. H. Padmasri;A. Venugopal
通讯作者：
V. Krishna;G. Naresh;Vikas Kumar;R. Sarkari;A. H. Padmasri;A. Venugopal