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Synthesis of high stability nanosized Rh/CeO2–ZrO2 three-way automotive catalysts by Rh chemical state regulation
Journal of the Energy Institute ( IF 5.6 ) Pub Date : 2020-07-22 , DOI: 10.1016/j.joei.2020.07.005
Yusheng Chen , Jun Fan , Jie Deng , Xue Jiang , Yi Jiao , Yaoqiang Chen

The chemical state of precious metals plays an important role in redox reaction. In order to maintain rhodium (Rh) at metallic state, which is recognized as reactive center in three-way catalytic reactions, we synthesized Rh/CeO2–ZrO2 (Rh/CZ) catalyst by liquid phase reduction adsorption with glycerol as reductant (Rh/CZ-g). Detailed characterizations were conducted to investigate the chemical state of Rh species, and the CO-FTIR and XPS results indicated that Rh species mainly existed in metallic state for Rh/CZ-g. Through CO chemisorption and H2-TPR, it's proved that the liquid phase reduction treatment would weaken the interaction between Rh species and CeO2–ZrO2 support, avoiding the supply of oxygen species from CeO2–ZrO2 to Rh in some degree. Compared with Rh/CeO2–ZrO2 catalyst prepared by incipient wetness impregnation, Rh/CZ-g exactly had superior activity in three-way catalytic process. Combined with in situ DRIFTS, some important intermediate species, such as Rh–CN, Rh-(NO)2, formates and acetates, preferred to adsorb and transform on Rh/CZ-g with larger proportion of metallic Rh, which determined Rh/CZ-g was more favorable for three-way catalytic reactions, even after aged at 950 °C for 5 h. The purpose of this work is to inspire researchers use simple and valid methods to synthesize highly efficient three-way catalysts.



中文翻译:

Rh化学态调控合成高稳定性纳米Rh / CeO 2 -ZrO 2三元汽车催化剂。

贵金属的化学状态在氧化还原反应中起重要作用。为了将铑(Rh)保持在金属状态(在三元催化反应中被认为是反应中心),我们通过以甘油为还原剂的液相还原吸附法合成了Rh / CeO 2 -ZrO 2(Rh / CZ)催化剂( Rh / CZ-g)。进行了详细的表征以研究Rh的化学状态,CO-FTIR和XPS结果表明Rh / CZ-g主要以金属态存在。通过CO的化学吸附和H 2 -TPR,证明了液相还原处理会减弱Rh物种与CeO 2 -ZrO 2的相互作用。支持,一定程度上避免了从CeO 2 -ZrO 2到Rh的氧供应。与初湿浸渍法制得的Rh / CeO 2 -ZrO 2催化剂相比,Rh / CZ-g在三元催化过程中确实具有优越的活性。与原位DRIFTS结合使用,一些重要的中间物种,例如Rh–CN,Rh-(NO)2,甲酸盐和乙酸盐,更倾向于吸附和转化具有较大比例的金属Rh的Rh / CZ-g,这决定了Rh / CZ-g对三元催化反应更有利,即使在950°C下老化5小时也是如此。这项工作的目的是激发研究人员使用简单有效的方法来合成高效的三效催化剂。

更新日期:2020-07-22
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