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首页> 外文期刊>Catalysis science & technology >Enhancement in catalytic performance of birnessite-type MnO2-supported Pd nanoparticles by the promotional role of reduced graphene oxide for toluene oxidation
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Enhancement in catalytic performance of birnessite-type MnO2-supported Pd nanoparticles by the promotional role of reduced graphene oxide for toluene oxidation

机译：通过还原氧化石墨烯对甲苯氧化的促销作用，Birnessite型MNO2支持的PD纳米颗粒的催化性能增强了催化性能

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Birnessite-type MnO2 (δ-MnO2)-supported reduced graphene oxide (rGO)-promoted palladium (xPd–yrGO/δ-MnO2) samples were prepared using a polyvinyl alcohol-protected reduction method. The physicochemical properties of the catalysts were determined by means of numerous techniques, and their catalytic activities for the oxidation of toluene were evaluated. It was found that the introduction of rGO as an electron transfer bridge could significantly strengthen the metal–support interaction (SMSI) between Pd and δ-MnO2, thereby enhancing the catalytic activity of the sample. Among all of the xPd–yrGO/δ-MnO2 samples, 0.48Pd–1.0rGO/δ-MnO2 performed the best: the toluene oxidation rates were 3.41 × 10−4 and 6.13 × 10−4 mol g−1 s−1 at 177 and 189 °C, respectively, with a space velocity of 60 000 mL g−1 h−1, which were much higher than that of 0.45Pd/δ-MnO2 at similar temperatures. The doping of rGO led to an increase in the Mn3+/Mn4+ or Oads/Olatt molar ratio, thus enhancing the catalytic activity of Pd/δ-MnO2. The good performance of 0.48Pd–1.0rGO/δ-MnO2 was associated with its high Oads/Olatt molar ratio, good low-temperature reducibility, and strong interaction between Pd and δ-MnO2. In situ DRIFTS results revealed that benzaldehyde and benzoate were the intermediate products of toluene oxidation over 0.48Pd–1.0rGO/δ-MnO2. The physicochemical properties of the 0.48Pd–1.0rGO/δ-MnO2 sample were not changed significantly after 70 h of stability test, but the activity of this catalyst decreased in the presence of CO2, SO2 or NH3, which was due to the carbonate, sulfate and ammonia species formed on the surface of 0.48Pd–1.0rGO/δ-MnO2 that covered the active sites and oxygen vacancies and thereby reduced the ability to bind with toluene.
机译：使用聚乙烯基醇保护的还原法制备了birnessite-type MNO2（δ-MNO2） - 支持的还原的氧化石墨烯（RGO）促成的钯（XPD – ERGO/δ-MNO2）样品。催化剂的物理化学特性是通过多种技术确定的，并评估了它们用于氧化的催化活性。发现将RGO作为电子传输桥的引入可以显着增强PD和δ-MNO2之间的金属 - 支撑相互作用（SMSI），从而增强样品的催化活性。在所有XPD – ERGO/δ-MNO2样品中，0.48pd – 1.0rgo/δ-MNO2的表现最好：甲苯氧化速率为3.41×10-4和6.13×10-4 mol G-1 s-1 s-1 AT 177和189°C分别为60 000 mL G-1 H-1，在类似温度下远高于0.45pd/δ-MNO2。 RGO的掺杂导致MN3+/MN4+或OADS/OLATT摩尔比增加，从而增强了PD/δ-MNO2的催化活性。 0.48pd – 1.0rgo/δ-MNO2的良好性能与其高OADS/OLATT摩尔比，良好的低温降低性以及PD和δ-MNO2之间的强相互作用有关。原位漂移结果表明，苯甲醛和苯甲酸酯是甲苯氧化超过0.48pd – 1.0rgo/δ-MNO2的中间产物。在稳定性测试70小时后，0.48pd – 1.0rgo/δ-MNO2样品的物理化学性质没有显着更改，但是在存在CO2，SO2或NH3的存在下，该催化剂的活性降低，这是由于碳酸盐，碳酸盐，碳酸盐造成的，在0.48pd – 1.0rgo/δ-MNO2表面形成的硫酸盐和氨种，覆盖了活性位点和氧空位，从而降低了与甲苯结合的能力。

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