A comparative IR characterization of acidic sites on HY zeolite by pyridine and CO probes with silica-alumina and γ-alumina references

被引:96
作者
Kondo, Junko N. [1 ]
Nishitani, Ryoko [1 ]
Yoda, Eisuke [2 ]
Yokoi, Toshiyuki [1 ]
Tatsumi, Takashi [1 ]
Domen, Kazunari [3 ]
机构
[1] Tokyo Inst Technol, Chem Resources Lab, Midori Ku, Yokohama, Kanagawa 2268503, Japan
[2] Univ Yamanashi, Grad Sch Med & Engn, Kofu, Yamanashi 4008511, Japan
[3] Univ Tokyo, Sch Engn, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
关键词
TEMPERATURE-PROGRAMMED DESORPTION; NUCLEAR-MAGNETIC-RESONANCE; AMORPHOUS SILICA; Y-ZEOLITE; INFRARED-SPECTROSCOPY; ADSORBED PYRIDINE; CARBON-MONOXIDE; HYDROXYL-GROUPS; SOLID-STATE; NMR;
D O I
10.1039/c0cp00203h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Using IR spectroscopy, three different surface states of HY zeolite were probed by successive adsorption of CO at 143 K followed by evacuation and pyridine adsorption at 523 K: HY zeolite [1] without strong Lewis acid sites (LAS); [2] after high temperature (873 K) evacuation to convert Bronsted acid sites (BAS) to strong LAS; and [3] after water re-adsorption on HY zeolite [2] to recover BAS from LAS. The original surface of HY zeolite [1] seemed to be recovered on HY zeolite [3] after high temperature evacuation and water treatment by CO adsorption, while a part of generated LAS on HY zeolite [2] seemed irreversible on HY zeolite [3] to HY zeolite [1] by pyridine adsorption. To clarify this discrepancy, re-examination of the IR spectra of adsorbed CO and pyridine on gamma-alumina and silica-alumina after similar treatments to those on HY zeolite was conducted. Based on the results of CO adsorption on gamma-alumina and silica-alumina, the presence of extra-framework aluminium sites on HY zeolite [1] was confirmed. High temperature evacuation of HY zeolite [1] formed very strong LAS, a part of which was irreversible to BAS by water re-adsorption at room temperature. The irreversible sites on HY zeolite [3] were assigned to non-acidic OH groups attributed to silica-alumina. The non-acidic OH groups on HY zeolite [3], which were BAS on HY zeolite [1], hydrogen-bonded to pyridine to show IR spectra similar to those adsorbed on LAS. Thus, LAS on HY zeolite [3] seemed irreversible by pyridine adsorption after water re-adsorption. On the other hand, CO adsorbed on non-acidic OH groups showed a band at only slightly lower frequency (2160 cm(-1)) than that of BAS (2178 cm(-1)), resulting in overlapps and ignoring their presence. Thus, CO adsorption seemed to show that complete recovery of LAS to BAS occurred.
引用
收藏
页码:11576 / 11586
页数:11
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