摘要
通过CeZr-BTC和CeNi-BTC双金属MOFs材料为前驱体制备了多孔CeNiOx和CeZrOx复合金属氧化物,并考察了对Pd组分的分散热稳定性及天然气燃料汽车(NGVs)三效催化性能改善的构效关系。试验结果表明,制备的负载型1%Pd/CeNiOx和1%Pd/CeZrOx催化剂上Pd组分分散度可分别达到约46.3%和39.9%,经800 ℃和8 h空气气氛下老化后Pd物种粒子大小分别约为5.7 nm和7.3 nm,仍表现出较好的分散粒度和储氧性能。相对地,Pd/CeNiOx催化剂上Pd物种粒子稳定性更佳,催化剂的储氧量也更高,老化后的模拟NGVs尾气三效净化催化低温活性更佳,尤其是NO和CH4催化转化性能更优,CO,NO和CH4的转化温度T50分别可达120,206,370 ℃,T90别可达180,330,480 ℃,但CH4的转化温度仍偏高。通过具有丰富孔道结构的MOFs材料来衍生制备复合金属氧化物载体,可以适度改善Pd组分的分散热稳定性,并提供更多的可吸附位点和氧空位,从而改善NGVs三效催化性能。
Abstract
The porous CeNiOx and CeZrOx composite metal oxides were prepared by using CeZr-BTC and CeNi-BTC bimetallic MOFs materials as precursor and the structureactivity relationship of improving the thermal stability of Pd component dispersion and the three-way catalytic performance of natural gas vehicles(NGVs) was investigated. The experimental results showed that the dispersions of Pd components on the prepared supported 1%Pd/CeNiOx and 1%Pd/CeZrOx catalysts reached about 46.3% and 39.9% respectively. The particle sizes of Pd species were about 5.7 nm and 7.3 nm and the catalysts still showed the better disperse particle sizse and oxygen-carrying properties after the aging of 800 ℃ and 8 h. Relatively, Pd particles on Pd/CeNiOx catalyst had the better stability and higher oxygen storage, and after aging the three-way purification of simulated NGVs exhaust had the better lowtemperature catalytic activity, especially for NO and CH4. The respective conversion temperature of CO, NO and CH4 conversion could reach 120 ℃, 206 ℃ and 370 ℃ for T50 and 180 ℃, 330 ℃ and 480 ℃ for T90, and the conversion temperature of CH4 was still too high. Accordingly, the preparation of composite metal oxide carrier derived from MOFs material with pore-rich structure could moderately improve the thermal stability of Pd component dispersion and provide more adsorption sites and oxygen vacancies and finally improve the threeway catalytic performance of NGVs exhaust.
关键词
天然气汽车 /
催化剂 /
制备 /
催化活性 /
稳定性
Key words
NG vehicle /
catalyst /
preparation /
catalytic activity /
stability
杨佳豪,岳焮羽,廖万年,刘来君,唐富顺.
MOFs衍生复合氧化物载体上Pd组分分散性与NGVs尾气催化净化性能[J]. 车用发动机. 2023, 0(4): 29-36 https://doi.org/10.3969/j.issn.1001-2222.2023.04.005
YANG Jiahao,YUE Xinyu,LIAO Wannian,LIU Laijun,TANG Fushun.
Dispersion of Pd Component on MOFs-Derived Composite Oxide Carrier and Catalytic Purification of NGVs Exhaust[J]. Vehicle Engine. 2023, 0(4): 29-36 https://doi.org/10.3969/j.issn.1001-2222.2023.04.005
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