Abstract

Dehydrogenation of ethane to ethylene was investigated in the presence of CO2 over Au catalyst supported on an Mn-doped ceria nanorod. The activity can be greatly enhanced by proper Mn doping. Mn was found to preferentially occupy defect sites or surface sites of ceria, resulting in the formation of extra oxide ions. Characterization results indicated that the reducible oxygen species related to ceria might play a vital role in the dehydrogenation. The addition of CO2 improved the stability of the catalysts remarkably, since CO2 can sustainably replenish the reducible oxygen species and eliminate the coke on the surface of the catalysts, which was proved by the H2-TPR and Raman analysis of spent catalysts. An ethane conversion of 17.4% with an ethylene selectivity of 97.5% can be obtained after 44 h of reaction.

Highlights

  • Being one of the most important types of compounds in the chemical industry, ethylene can be extensively used as feedstock for producing polyethylene, ethylene oxide, ethylene glycol, vinyl chloride, acetaldehyde, acetic acid and other derivates

  • Dry reforming as well as oxidative dehydrogenation can occur over these supported Au catalysts

  • Previous studies have shown that this CeO2 nanorod grows along the results reported before

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Summary

Introduction

Being one of the most important types of compounds in the chemical industry, ethylene can be extensively used as feedstock for producing polyethylene, ethylene oxide, ethylene glycol, vinyl chloride, acetaldehyde, acetic acid and other derivates. Cr2 O3 - and Ga2 O3 -based catalysts are reported to be more active than others for the reaction [7,8,9,10,11]. These kinds of catalysts are still limited by the drawbacks of environmental hostility, relatively low selectivity or poor long-term stability. The reaction between ethane/propane and CO2 has been studied on Au-based catalysts [12,13]. More recent results show that CeO2 -supported Au is an excellent catalyst for oxidative dehydrogenation of ethane with CO2 , and nanorod CeO2 -supported Au exhibits higher activity and better stability than nanoparticle supported one [14]. The surface oxygen reducibility of ceria is found to play a vital role in dehydrogenation

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