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Understanding the Active Sites of Ag/Zeolites and Deactivation Mechanism of Ethylene Catalytic Oxidation at Room Temperature
ACS Catalysis ( IF 12.9 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acscatal.7b02410
Hongling Yang 1, 2 , Chunyan Ma 1, 2 , Xin Zhang 1, 2 , Yang Li 1 , Jie Cheng 1, 2 , Zhengping Hao 1, 2
Affiliation  

Microporous Ag/zeolite (ZSM-5, Beta, Y, and Mordenite) catalysts were found to be potentially good catalytic materials for ethylene oxidation at room temperature. These catalysts were evaluated under both dry and humid atmospheres, achieving 100% conversion of 100 ppm of ethylene mineralized into CO2 at 25 °C. Moreover, the zeolite framework type and relative humidity had a significant effect on catalytic stability. Pyridine Fourier transform infrared spectra (FTIR) and solid-state hydrogen-1 (1H) magic angle spinning nuclear magnetic resonance (MAS NMR) studies revealed that Brønsted acid sites were the active sites in Ag/zeolites; the deactivated Ag/zeolites had no available Brønsted acid sites. When the number of Brønsted acid sites of Ag/ZSM-5-humid and Ag/Beta-humid were reduced, the catalytic activities of Ag/ZSM-5-humid and Ag/Beta-humid decreased. Temperature-programmed oxidation mass spectrometry (TPO-MS) and water adsorption/desorption results indicated that H2O adsorbed on Brønsted acid sites led to the disappearance of available Brønsted acid sites and thus resulted in Ag/zeolite catalyst deactivation. An understanding of the active sites and deactivation mechanism in ethylene oxidation on zeolite catalysts is helpful in the synthesis of a better ethylene oxidation catalyst and development of an effective technology of eliminating trace ethylene.

中文翻译:

了解Ag /沸石的活性位点和室温下乙烯催化氧化的失活机理

发现微孔银/沸石(ZSM-5,β,Y和丝光沸石)催化剂是室温下乙烯氧化的潜在良好催化材料。在干燥和潮湿的气氛下对这些催化剂进行了评估,在25°C下实现了100 ppm的乙烯矿化成CO 2的100%转化。而且,沸石骨架类型和相对湿度对催化稳定性有显着影响。吡啶傅里叶变换红外光谱(FTIR)和固态氢-1(1H)魔角旋转核磁共振(MAS NMR)研究表明,布朗斯台德酸位点是Ag /沸石中的活性位点;失活的Ag /沸石没有可用的布朗斯台德酸位。当减少Ag / ZSM-5-湿润和Ag / Beta湿润的布朗斯台德酸中心数目时,Ag / ZSM-5-湿润和Ag / Beta湿润的催化活性降低。程序升温氧化质谱(TPO-MS)和水吸附/解吸结果表明H 2吸附在布朗斯台德酸性位点上的O导致可用的布朗斯台德酸性位点消失,从而导致Ag /沸石催化剂失活。了解沸石催化剂上乙烯氧化的活性位和失活机理,有助于合成更好的乙烯氧化催化剂和开发消除痕量乙烯的有效技术。
更新日期:2018-01-17
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