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Deactivation behaviour of supported gold palladium nanoalloy catalysts during the selective oxidation of benzyl alcohol in a micro-packed bed reactor

机译:微填充床反应器中苄醇选择性氧化过程中负载型金钯纳米合金催化剂的失活行为

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摘要

Highly active, supported Au-Pd catalysts have been tested for catalysing benzyl alcohol oxidation in a silicon-glass micro-packed bed reactor. The effects of Au-Pd composition and anion content during catalyst preparation on catalyst deactivation were studied, and a relationship between the deactivation rate and the amount of Cl- and Au used in the catalyst formulation was found. Whilst Au aids in enhancing the selectivity to the desired product and the Cl- ions help the formation of uniform 1-2 nm nanoparticles, higher amounts of Au and Cl- become detrimental to the catalyst stability once a certain amount is exceeded. Loss of small (1-2 nm) metal nanoparticles was evident in all catalysts studied, accompanied by agglomeration and the formation of larger >10nm particles. A secondary deactivation mechanism characterised by the formation of an amorphous surface film was observed via TEM in catalysts with high Cl- and Au and was confirmed by the detection of carbon species on the catalyst surface using Raman Spectroscopy.
机译:已经测试了高活性负载型Au-Pd催化剂在硅玻璃微填充床反应器中催化苯甲醇氧化的能力。研究了催化剂制备过程中Au-Pd的组成和阴离子含量对催化剂失活的影响,发现失活速率与催化剂配方中Cl-和Au的用量之间的关系。尽管Au有助于增强对所需产物的选择性,Cl-离子有助于形成均匀的1-2 nm纳米颗粒,但一旦超过一定量,更高数量的Au和Cl-就会损害催化剂的稳定性。在所有研究的催化剂中,小(1-2 nm)金属纳米颗粒的损失都是明显的,伴随着团聚和大于10nm的较大颗粒的形成。在具有高Cl-和Au的催化剂中,通过TEM观察到了以形成无定形表面膜为特征的二次失活机理,并通过使用拉曼光谱法检测了催化剂表面的碳物种得到了证实。

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