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稀土氧化物掺杂二氧化铈负载铜催化剂上乙酸乙酯的去除

Ethyl Acetate Abatement on Copper Catalysts Supported on Ceria Doped with Rare Earth Oxides.

作者信息

Carabineiro Sónia Alexandra Correia, Konsolakis Michalis, Marnellos George Emmanouil-Nontas, Asad Muhammad Faizan, Soares Olívia Salomé Gonçalves Pinto, Tavares Pedro Bandeira, Pereira Manuel Fernando Ribeiro, Órfão José Joaquim de Melo, Figueiredo José Luís

机构信息

Laboratório de Catálise e Materiais (LCM), Laboratório Associado LSRE-LCM, Faculdade de Engenharia, Universidade do Porto, 4200-465 Porto, Portugal.

School of Production Engineering and Management, Technical University of Crete, 73100 Chania, Greece.

出版信息

Molecules. 2016 May 17;21(5):644. doi: 10.3390/molecules21050644.

DOI:10.3390/molecules21050644
PMID:27196886
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6273042/
Abstract

Different lanthanide (Ln)-doped cerium oxides (Ce0.5Ln0.5O1.75, where Ln: Gd, La, Pr, Nd, Sm) were loaded with Cu (20 wt. %) and used as catalysts for the oxidation of ethyl acetate (EtOAc), a common volatile organic compound (VOC). For comparison, both Cu-free (Ce-Ln) and supported Cu (Cu/Ce-Ln) samples were characterized by N₂ adsorption at -196 °C, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and temperature programmed reduction in H₂. The following activity sequence, in terms of EtOAc conversion, was found for bare supports: CeO₂ ≈ Ce0.5Pr0.5O1.75 > Ce0.5Sm0.5O1.75 > Ce0.5Gd0.5O1.75 > Ce0.5Nd0.5O1.75 > Ce0.5La0.5O1.75. Cu addition improved the catalytic performance, without affecting the activity order. The best catalytic performance was obtained for Cu/CeO₂ and Cu/Ce0.5Pr0.5O1.75 samples, both achieving complete EtOAc conversion below ca. 290 °C. A strong correlation was revealed between the catalytic performance and the redox properties of the samples, in terms of reducibility and lattice oxygen availability. Νo particular correlation between the VOC oxidation performance and textural characteristics was found. The obtained results can be explained in terms of a Mars-van Krevelen type redox mechanism involving the participation of weakly bound (easily reduced) lattice oxygen and its consequent replenishment by gas phase oxygen.

摘要

将不同的镧系元素（Ln）掺杂的氧化铈（Ce0.5Ln0.5O1.75，其中Ln为：Gd、La、Pr、Nd、Sm）负载20 wt.%的Cu，并用作氧化常见挥发性有机化合物（VOC）乙酸乙酯（EtOAc）的催化剂。为作比较，对无Cu（Ce-Ln）和负载Cu（Cu/Ce-Ln）的样品均采用-196℃下的N₂吸附、扫描/透射电子显微镜、能量色散X射线光谱、X射线衍射、X射线光电子能谱以及H₂程序升温还原进行表征。对于裸载体，发现就EtOAc转化率而言，其活性顺序如下：CeO₂≈Ce0.5Pr0.5O1.75＞Ce0.5Sm0.5O1.75＞Ce0.5Gd0.5O1.75＞Ce0.5Nd0.5O1.75＞Ce0.5La0.5O1.75。添加Cu提高了催化性能，但不影响活性顺序。Cu/CeO₂和Cu/Ce0.5Pr0.5O1.75样品的催化性能最佳，二者均在约290℃以下实现了EtOAc的完全转化。就样品的还原性和晶格氧可用性而言，催化性能与样品的氧化还原性质之间呈现出强烈的相关性。未发现VOC氧化性能与织构特征之间存在特定相关性。所得结果可以用涉及弱结合（易还原）晶格氧参与及其随后被气相氧补充的Mars-van Krevelen型氧化还原机理来解释。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/a086e91d56f2/molecules-21-00644-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/030e70055554/molecules-21-00644-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/5f1bacec6ba3/molecules-21-00644-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/2dfad7d7370f/molecules-21-00644-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/a8442960ca90/molecules-21-00644-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/2a941655aae6/molecules-21-00644-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/e3a0670c2c83/molecules-21-00644-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/97b3f5036249/molecules-21-00644-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/c556295f723c/molecules-21-00644-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/622f42b78946/molecules-21-00644-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/a086e91d56f2/molecules-21-00644-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/030e70055554/molecules-21-00644-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/5f1bacec6ba3/molecules-21-00644-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/2dfad7d7370f/molecules-21-00644-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/a8442960ca90/molecules-21-00644-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/2a941655aae6/molecules-21-00644-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/e3a0670c2c83/molecules-21-00644-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/97b3f5036249/molecules-21-00644-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/c556295f723c/molecules-21-00644-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/622f42b78946/molecules-21-00644-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c88/6273042/a086e91d56f2/molecules-21-00644-g010.jpg

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