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首页> 外文期刊>Catalysis science & technology >Zeolite-supported rhodium sub-nano cluster catalyst for low-temperature selective oxidation of methane to syngas
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Zeolite-supported rhodium sub-nano cluster catalyst for low-temperature selective oxidation of methane to syngas

机译:Zeolite-supported铑sub-nano集群低温选择性氧化的催化剂甲烷制合成气

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摘要

The conversion of methane to syngas under mild conditions is a key to efficiently utilise natural gas, including shale gas, in chemical industries. In this work, we demonstrate that Rh sub-nano clusters formed on zeolites catalyse the partial oxidation of methane to syngas at substantially lower temperatures (450-600 °C) than those required in previous reports (>700 °C). Rh sub-nano clusters of 0.6 nm diameter were prepared by a simple ion-exchange method. The catalyst gave 84% conversion of methane with 91% selectivity for CO and a H2/CO ratio of 2.0 at 600 °C even at a very high space velocity (1 200000 mL h~(-1) g~(-1)). No deactivation was observed in the durability test for 50 h, and the turnover number of bulk Rh for the formation of CO reached 2 600000. Kinetic and spectroscopic studies revealed that a combustion-reforming mechanism occurs on the metallic Rh sub-nano clusters. The acidity of the zeolite played no role in the reaction, but the ion-exchange properties of zeolites were crucial to prepare the active Rh catalysts.
机译:下的甲烷转化成合成气温和条件是高效利用的关键天然气,包括页岩气在内的化学物质行业。sub-nano集群形成沸石催化甲烷部分氧化制合成气大幅降低温度(450 - 600°C)比需要在之前的报告(> 700°C)。由一个简单的离子交换方法。催化剂给84%转化甲烷的91%选择性的CO和H2 / CO比率为2.0600°C即使在非常高的空间速度(1200000毫升h ~ (1) g ~(1))。耐久性试验中观察到50 h,周转率的散装Rh的形成公司达到了600000。研究表明,combustion-reforming发生在金属Rh sub-nano机制集群。在反应中的作用,但离子交换沸石的性质是至关重要的准备活跃的Rh催化剂。

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