A comparative first principles study on trivalent ion incorporated SSZ-13 zeolites

作者：Wen, Cui; Geng, Lu; Han, Lina; Wang, Jiancheng^*; Chang, Liping; Feng, Gang; Kong, Dejin; Liu, Jianwen

来源：Physical Chemistry Chemical Physics, 2015, 17(44): 29586-29596.

DOI：10.1039/c5cp04788a

• TOTAL-ENERGY CALCULATIONS
• BRONSTED ACID SITES
• HYDROXYL-GROUPS
• CHABAZITE
• CHA
• METHANOL
• CONVERSION
• AL
• ADSORPTION
• PROPENE

The dispersion-corrected density functional theory has been used to study the trivalent ions B, Al, Ga, and Fe incorporated SSZ-13-type zeolites. The associated structure and Bronsted/Lewis acidity change caused by the incorporation ions were comparatively studied. It was found that the smaller the radius differences of the incorporation ions are, the smaller the changes in the structure will be and the less acidity will be enhanced for the Bronsted sites. The trivalent Al is found to be the most favorable trivalent incorporation ion and Na is found to be the most favorable charge balanced ion for the synthesis of SSZ-13-type zeolites due to size comparability, which are in line with the experimental observation. The substitution energies which show the relative synthesis difficulty level were also applied for B, Al, Ga, and Fe incorporated zeolites and found that the difficulty decreases with order of Fe > B > Ga >> Al, also in good agreement with the experimental observations. Adsorption studies for the NH3 and pyridine molecules indicate that adsorption on the Bronsted acid sites is more stable than on the Lewis acid sites. The Bronsted acidity was found to follow the order of HAl-SSZ-13 > HGa-SSZ-13 approximate to HFe-SSZ-13 > HB-SSZ-13 where the Lewis acidity was found to follow the order of HGa-SSZ-13 approximate to HFe-SSZ-13 > HAl-SSZ-13 > HB-SSZ-13. Our results provide new insights for the synthesis of the SSZ-13-type zeolites and fundamental information for the zeolitic catalyst designation to enhance the catalytic performance.

• 出版日期2015
• 单位国家超级计算深圳中心; 中国石油化工股份有限公司上海石油化工研究院; 南昌大学; 太原理工大学