Suppr超能文献

采用硅铝酸和γ-氧化铝参比物,通过吡啶和 CO 探针对 HY 沸石酸性位进行比较红外光谱表征。

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

机构信息

Chemical Resources Laboratory, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan.

出版信息

Phys Chem Chem Phys. 2010 Oct 7;12(37):11576-86. doi: 10.1039/c0cp00203h. Epub 2010 Aug 3.

Abstract

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 Brønsted 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 γ-alumina and silica-alumina after similar treatments to those on HY zeolite was conducted. Based on the results of CO adsorption on γ-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.

摘要

使用红外光谱法,通过在 143 K 下连续吸附 CO,然后在 523 K 下抽真空和吸附吡啶,研究了 HY 沸石的三种不同表面状态:[1] 没有强路易斯酸位(LAS)的 HY 沸石;[2] 经过高温(873 K)抽真空将 Brønsted 酸位(BAS)转化为强 LAS;[3] 在 HY 沸石[2]上重新吸附水以 LAS 从 BAS 中恢复。HY 沸石[1]的原始表面在高温抽真空和 CO 吸附处理后似乎在 HY 沸石[3]上得到恢复,而 HY 沸石[2]上生成的一部分 LAS 在 HY 沸石[3]上似乎对 HY 沸石[1]不可逆,通过吡啶吸附。为了澄清这种差异,对 HY 沸石进行类似处理后吸附在γ-氧化铝和硅铝酸钙上的 CO 和吡啶的红外光谱进行了重新检查。基于 CO 在γ-氧化铝和硅铝酸钙上的吸附结果,证实了 HY 沸石[1]中存在骨架外铝位。HY 沸石[1]的高温抽真空形成了非常强的 LAS,其中一部分 LAS 通过室温下重新吸附水而不可逆地转化为 BAS。HY 沸石[3]上不可逆的位点被分配到非酸性 OH 基团归因于硅铝酸钙。HY 沸石[3]上的非酸性 OH 基团在 HY 沸石[1]上是 BAS,与吡啶形成氢键,表现出与吸附在 LAS 上相似的红外光谱。因此,HY 沸石[3]上的 LAS 在重新吸附水后通过吡啶吸附似乎不可逆。另一方面,吸附在非酸性 OH 基团上的 CO 在稍低的频率(2160 cm(-1))下显示出一个带,低于 BAS(2178 cm(-1)),导致重叠并忽略其存在。因此,CO 吸附似乎表明 LAS 完全恢复到 BAS。

文献AI研究员

20分钟写一篇综述,助力文献阅读效率提升50倍。

立即体验

用中文搜PubMed

大模型驱动的PubMed中文搜索引擎

马上搜索

文档翻译

学术文献翻译模型,支持多种主流文档格式。

立即体验