| 张嘉霖,孙培永,张胜红,姚志龙.乙烯催化转化制备乙二醇反应中TS-1分子筛的失活[J].分子催化(中英文),2015,(3):229-237 |
| 乙烯催化转化制备乙二醇反应中TS-1分子筛的失活 |
| Deactivation of TS-1 Zeolites in the Catalytic Conversion of Ethylene to Ethylene Glycol |
| 投稿时间：2015-05-07 修订日期：2015-06-08 |
| DOI： |
| 中文关键词: 乙烯 乙二醇 TS-1分子筛 失活 再生 |
| 英文关键词:Ethylene Ethylene glycol TS-1 zeolites Deactivation Regeneration |
| 基金项目:北京市自然科学基金 |
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| 摘要点击次数: 1831 |
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| 中文摘要: |
| 采用连续循环反应的方式考察了TS-1分子筛在催化双氧水氧化乙烯制备乙二醇反应中的失活过程。其中，新鲜、反应后和再生的TS-1分子筛采用氮气物理吸附、XRF、SEM、XRD、FT-IR和UV-vis等技术进行表征，反应后分子筛表面的吸附物种分别采用FT-IR、GC-MS和TG-DTA进行定性和定量分析。结果表明，反应过程中TS-1分子筛未发生明显的Ti物种的流失，乙二醇低聚物等大分子有机物在分子筛微孔通道内的聚集而引起的孔道堵塞和活性Ti位点可及度的降低是分子筛部分失活的主要原因。失活后的催化剂可以通过双氧水处理移除其表面吸附的物种而部分再生, 而高温焙烧可以彻底清除分子筛孔道内沉积的有机物从而恢复分子筛的催化活性。 |
| 英文摘要: |
| Deactivation process of TS-1 zeolites in the catalytic conversion of ethylene to ethylene glycol in an aqueous solution of H2O2 was studied in detail. The fresh, used and regenerated TS-1 zeolites were carefully characterized by nitrogen physical adsorption, XRF, SEM, XRD, FT-IR and UV-vis spectra, and the adsorbed organic species on the used TS-1 catalysts were analyzed by using FT-IR, GC-MS and TG-DTA techniques. Characterization results indicated that the leaching of framework Ti species in reaction was negligible, and that partial deactivation of TS-1 zeolites in the consecutive cycling reactions was probably caused by the loss in the accessibility of active Ti sites, due to the blocking of micropore channels of TS-1 by the deposited organic oligomers. Treating the used TS-1 catalyst with an aqueous solution of H2O2 could remove most of the organic depositions and recover partly its catalytic activity. By contrast, calcination at 550 oC could clear thoroughly the deposited organics in the deactivated TS-1 catalysts, leading to an identical performance to that of the fresh TS-1 zeolites. |
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