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Pd-based catalysts promoted by hierarchical porous Al2O3 and ZnO microsphere supports/coatings for ethyl acetate highly active and stable destruction.
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2020-06-22 , DOI: 10.1016/j.jhazmat.2020.123281
Mudi Ma 1 , Rui Yang 1 , Chi He 2 , Zeyu Jiang 1 , Jian-Wen Shi 3 , Reem Albilali 4 , Khaled Fayaz 5 , Baojun Liu 6
Affiliation  

Developing economical and active materials is of great significance for VOC purification. Here, hierarchical porous Al2O3 and ZnO microspheres (Al2O3-pm and ZnO-pm) were synthesized by a facile hydrothermal strategy. The urchin-like Al2O3-pm and flower-like ZnO-pm possess high specific surface area (especially; external surface area) obviously boost the dispersion of Pd with 29.3 % and 30.1 % over Pd/Al2O3-pm and Pd/ZnO-pm, respectively, over 3.4 times higher than those of commercial Al2O3- and ZnO-supported counterparts. Pd/Al2O3-pm possesses excellent activity and CO2 yield in ethyl acetate (EA) degradation, with TOF reaches 7.76 × 10−3 s−1 at 160 °C under GHSV of 50,000 h-1. Moreover, Pd/Al2O3-pm exhibits satisfied performance in EA-contained binary VOCs oxidation and has high long-term stability under both dry and humid conditions. Both Pd sites and Brønsted acid sites participated in reaction process and initially react with EA to form ethylene and ethanol, respectively. Larger amount Brønsted acid sites over Pd/Al2O3-pm promote ethanol formation and C-C cleavage, resulting in different CO2 yields and EA activation mechanisms. The coating greatly enhances Pd dispersion over Pd supported monolithic catalyst, endowing its desired activity and stability even with a much lower Pd loading. This work promotes the potential application of noble-metal-based monolithic materials in VOC degradation.



中文翻译:

分层多孔Al2O3和ZnO微球载体/涂层促进的基于Pd的催化剂对乙酸乙酯具有高活性和稳定的破坏作用。

开发经济有效的材料对VOC的净化具有重要意义。在此,通过简便的水热策略合成了分层的多孔Al 2 O 3和ZnO微球(Al 2 O 3 -pm和ZnO-pm)。海胆状的Al 2 O 3 -pm和花状的ZnO-pm具有较高的比表面积(特别是外表面积),与Pd / Al 2 O 3 -pm相比,Pd的分散性提高了29.3%和30.1%。和Pd / ZnO-pm分别比市售Al 2 O 3和ZnO负载的对应物高3.4倍以上。钯/铝2 O 3-PM具有优异的活性和CO 2产率在乙酸乙酯(EA)的降解,用TOF达到7.76×10 -3小号-1在160℃下GHSV为50,000ħ -1。此外,Pd / Al 2 O 3 -pm在含有EA的二元VOCs氧化中表现出令人满意的性能,并且在干燥和潮湿条件下均具有很高的长期稳定性。Pd位和Brønsted酸位都参与了反应过程,并最初与EA反应分别形成乙烯和乙醇。Pd / Al 2 O 3 -pm上的大量布朗斯台德酸中心促进乙醇形成和CC裂解,从而导致不同的CO 2产量和EA激活机制。该涂层大大增强了Pd在负载Pd的整体催化剂上的分散性,即使在Pd含量低得多的情况下,仍具有所需的活性和稳定性。这项工作促进了贵金属单块材料在VOC降解中的潜在应用。

更新日期:2020-07-03
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