Preparation of the surface Ti, Al rich ETS-10 and modification of its pore structure and acidity by desilication and realumination
Preparation of the surface Ti, Al rich ETS-10 and modification of its pore structure and acidity by desilication and realumination
复制标题
表面富Ti、Al ETS-10的制备及其孔结构和酸度的脱硅、再铝改性
DOI：
10.1016/j.micromeso.2011.06.034
复制
发表时间：
2011-11
影响因子：
5.2
通讯作者：
中科院分区：
文献类型：
--
作者：
通过脱硅和再铝的连续过程获得表面富钛（Ti）和富铝（Al）的ETS-10。结合X射线光电子能谱（XPS）和X射线荧光（XRF）分析证实，ETS-10骨架中的部分硅（Si）原子通过脱硅被去除，导致Ti原子在ETS-10中富集。体Si/Ti原子比从4.6降低到4.2，并且表面Si/Ti原子比从9.1降低到5.5。氮气吸附-脱附分析表明，随着脱硅过程的进行，ETS-10的孔隙率沿着提高，其中最显著的是介孔体积从0.022 cm 3/g增加到0.085 cm 3/g。孔隙率的提高有利于Al原子的引入，为合金提供了额外的空间，经ETS-10再渗铝后，体相Al/Ti原子比达到0.4，表面相Al/Ti原子比达到1.9。27 Al MAS NMR结果表明，ETS-10中引入的Al原子大多以四面体配位，形成Si-（OH）-Al位的桥连羟基，形成沸石型酸性。通过FT-IR分析，结合氨程序升温脱附（NH3-TPD）和吡啶（Py）吸附，证明ETS-10的酸性得到了改善。强Brönsted酸中心和强刘易斯酸中心同时增加。采用异丙苯裂解反应考察了含铝ETS-10的酸性，在673 K时，异丙苯转化率比合成的ETS-10提高了18%。
The surface titanium (Ti) and aluminium (Al) rich ETS-10 was obtained by sequential processes of desilication and realumination. Combined X-ray photoelectron spectroscopy (XPS) and X-ray fluorescence (XRF) analysis confirmed that a part of silicon (Si) atoms in the framework of ETS-10 were removed via desilication which resulted in the enrichment of Ti atoms in ETS-10. The bulk Si/Ti atom ratio was decreased from 4.6 to 4.2, and the surface Si/Ti atom ratio was decreased from 9.1 to 5.5. Nitrogen adsorption–desorption analysis showed that the porosity of ETS-10 was improved along with the desilication process, and the most remarkable improvement was that the mesoporous volume was increased from 0.022cm3/g to 0.085cm3/g. The improved porosity facilitated the incorporation of Al atoms by supplying additional space, and with the processing of realumination to ETS-10, the bulk phase Al/Ti atom ratio reached to 0.4 and the surface phase Al/Ti atom ratio reached to 1.9. The results of27Al MAS NMR pointed out that the majority of the Al atoms introduced to ETS-10 were tetrahedrally coordinated and thus generating bridging hydroxyl groups of Si–(OH)–Al sites for zeolite-type acidity. The acidity of ETS-10 was improved after realumination, which was concluded by the combined ammonia temperature-programmed desorption (NH3-TPD) and pyridine (Py) adsorption performed via FT-IR analysis. The strong Brönsted and Lewis acid sites were increased together. Cumene cracking reaction was employed to test the acidity properties of Al-containing ETS-10, and the cumene conversion increased by 18% at 673K compared with the as-synthesized ETS-10.
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影响因子：
3.9
作者：
G. Zhao;Jia Lee;P. A. Chia
通讯作者：
G. Zhao;Jia Lee;P. A. Chia
影响因子：
2.8
作者：
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通讯作者：
Andreas Philippou;J. Rocha;Michael W Anderson
DOI：
10.1016/s0927-6513(97)00011-4
发表时间：
1997-07-01
期刊：
MICROPOROUS MATERIALS
影响因子：
--
作者：
Liepold, A;Roos, K;Anderson, MW
通讯作者：
Anderson, MW
影响因子：
7.3
作者：
Xie Zai-ku;Bao Jia-qing;Yang Yiqing;Chen Qing-ling;Zhang Chengfang
通讯作者：
Xie Zai-ku;Bao Jia-qing;Yang Yiqing;Chen Qing-ling;Zhang Chengfang
影响因子：
15
作者：
S. Ganapathy;T. Das;R. Vetrivel;S. S. Ray-S.;T. Sen;S. Sivasanker;L. Delevoye;C. Fernandez;J. Amoureux
通讯作者：
S. Ganapathy;T. Das;R. Vetrivel;S. S. Ray-S.;T. Sen;S. Sivasanker;L. Delevoye;C. Fernandez;J. Amoureux