Catalytic performance and stability of Fe-doped CeO2 in propane oxidative dehydrogenation using carbon dioxide as an oxidant,Catalysis Science & Technology

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Catalytic performance and stability of Fe-doped CeO2 in propane oxidative dehydrogenation using carbon dioxide as an oxidant
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-06-01 , DOI: 10.1039/d0cy00586j
Hedun Wang _{1,

2,

3,

4} , George Tsilomelekis _{1,

2,

3,

4}

Affiliation

Propane oxidative dehydrogenation (ODH) in the presence of CO₂ was investigated over a series of Fe-doped CeO₂ catalysts. The well-recognized properties of cerium oxide materials regarding improved oxygen mobility and oxygen storage capacity (OSC) were utilized towards the synthesis of stable catalytic systems. The iron–cerium oxide solid solution catalysts with an Fe dopant content from 1% up to 15% were successfully synthesized via a co-precipitation method and calcined at 873 K. It was confirmed by XRD and Raman characterization that all samples featured a single cerianite crystalline phase with periodic lattice Ce ions substituted by Fe ions, with no hematite phase identified. Initial screening of catalytic behavior showed that the propane ODH pathway was enhanced at high Fe/Ce ratio while propane cracking was suppressed. Stable propane conversion and propylene selectivity for up to 20 hours were achieved for the synthesized catalysts with moderate Fe loading. Ex situ Raman, XPS and STEM were applied to analyze post-reaction catalysts and confirmed that deactivation occurring over low Fe catalysts resulted from coke deposition on the surface, while CeO₂ sintering and Fe migration to form nanocrystals were the primary deactivation reasons for high Fe loading catalysts.

中文翻译：

Fe掺杂CeO2在以二氧化碳为氧化剂的丙烷氧化脱氢中的催化性能和稳定性

在一系列Fe掺杂的CeO ₂催化剂上研究了在CO ₂存在下的丙烷氧化脱氢（ODH）。氧化铈材料关于改善的氧迁移率和氧存储能力（OSC）的公认特性被用于合成稳定的催化体系。Fe掺杂含量从1％到15％的铁-铈氧化物固溶体催化剂已成功通过一种共沉淀法，在873 K下煅烧。通过XRD和Raman表征证实，所有样品均具有单片陶粒晶相，其中周期性晶格Ce离子被Fe离子取代，未鉴定到赤铁矿相。初步筛选的催化行为表明，在高Fe / Ce比下，丙烷ODH途径得到增强，而丙烷裂解受到抑制。对于合成的具有中等铁负载量的催化剂，丙烷的转化率和丙烯选择性长达20小时。使用异位拉曼光谱仪，XPS和STEM分析后反应催化剂，并确认低铁催化剂上发生的失活是由于表面上的焦炭沉积，而CeO ₂ 烧结和铁迁移形成纳米晶体是高铁负载催化剂失活的主要原因。

更新日期：2020-07-06

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