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Development of a Cs-Ru/CeO2 Spherical Catalyst Prepared by Impregnation and Washing Processes for Low-Temperature Decomposition of NH3: Characterization and Kinetic Analysis Results
Industrial & Engineering Chemistry Research ( IF 4.2 ) Pub Date : 2020-09-22 , DOI: 10.1021/acs.iecr.0c03112
Takeshi Furusawa 1, 2 , Hiroki Kuribara 1 , Koji Kimura 2 , Takafumi Sato 1, 2 , Naotsugu Itoh 1
Affiliation  

Cl-free Ru/CeO2 spherical catalysts were prepared by incipient wetness impregnation and subsequent washing processes using RuCl3·3H2O and a commercial spherical CeO2 support. Cs addition improved the catalytic performance for NH3 decomposition, and the optimal Cs loading was a Cs/Ru molar ratio of 0.43. Transmission electron microscopy (TEM) and scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM–EDX) suggested that Cs was present around Ru metal particles and served as an anchor for forming small, well-dispersed Ru metal particles (∼2 nm). CO2 temperature-programmed desorption results indicated that the Cs-Ru/CeO2 catalyst had more strong basic sites than the Ru/CeO2 catalyst. Kinetic analysis results clearly demonstrated that Cs addition promoted recombinative desorption of N atoms, which is the rate-determining step of NH3 decomposition. Consequently, the Cs-Ru/CeO2 spherical catalyst (Cs/Ru = 0.43) treated in Ar for 1 h at 773 K exhibited high catalytic activity for NH3 decomposition (NH3 conversion: 40% at 523 K and 80% at 573 K) at 2000 mL-NH3 g cat–1 h–1.

中文翻译:

NH 3低温分解浸渍和洗涤工艺制备的Cs-Ru / CeO 2球形催化剂的表征和动力学分析

通过初湿浸渍和随后的洗涤过程,使用RuCl 3 ·3H 2 O和商业球形CeO 2载体,制备了无Cl Ru / CeO 2球形催化剂。Cs的添加改善了NH 3分解的催化性能,并且最佳的Cs负载量为0.43的Cs / Ru摩尔比。透射电子显微镜(TEM)和扫描电子显微镜以及能量色散X射线光谱(SEM–EDX)表明,铯存在于Ru金属粒子周围,并作为形成细小,分散良好的Ru金属粒子的锚点(〜2 nm)。CO 2程序升温程序解吸结果表明,Cs-Ru / CeO 2催化剂具有比Ru / CeO 2催化剂更强的碱性位点。动力学分析结果清楚地表明,Cs的添加促进了N原子的重组解吸,这是NH 3分解的速率决定步骤。因此,在773 K下在Ar中处理1 h的Cs-Ru / CeO 2球形催化剂(Cs / Ru = 0.43)对NH 3分解显示出高催化活性(NH 3转化率:523 K为40%,573为80%)。 K)在2000 mL-NH 3 g cat –1 h –1
更新日期:2020-10-15
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