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Effect of CO2 Co-Feeding on the Stabilization of Atomically Dispersed Iron Species over MgAl2O4 During Ethane Dehydrogenation Reactions
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-08-08 , DOI: 10.1021/acscatal.3c02029 Yingbin Zheng 1, 2 , Junjie Li 1 , Xinbao Zhang 1 , Jie An 1 , Wenjie Xin 1 , Xiangxue Zhu 1 , Xiujie Li 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-08-08 , DOI: 10.1021/acscatal.3c02029 Yingbin Zheng 1, 2 , Junjie Li 1 , Xinbao Zhang 1 , Jie An 1 , Wenjie Xin 1 , Xiangxue Zhu 1 , Xiujie Li 1
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Ethane dehydrogenation provides an opportunity for the effective utilization of shale gas and production of ethene. Up to now, it is still a great challenge to acquire a stable ethane dehydrogenation catalyst operated under high temperature and reductive atmospheres. In this study, we prepared an Fe-based catalyst supported on MgAl2O4 with atomically dispersed iron species even after 6 reaction–regeneration cycles. Sheet-like morphology and spinel structure of MgAl2O4 is beneficial for the high dispersion of Fe species. The iron species undergoes reduction, sintering, and detachment during the ethane dehydrogenation reaction, as evidenced by in situ High-Angle Annular Dark-Field Scanning Transmission Electron Microscopy and quasi-in situ 57Fe Mössbauer spectroscopy. By contrast, the introduction of CO2 leads to a slow deactivation, where only the partial reduction of isolated Fe3+ species to isolated Fe2+ species was observed. And the activity could be restored by a simple O2 treatment. The current work sheds light on the design of high-efficient dehydrogenation catalysts.
中文翻译：
乙烷脱氢反应过程中 CO2 共进料对 MgAl2O4 上原子分散铁物种稳定性的影响
乙烷脱氢为页岩气的有效利用和生产乙烯提供了机会。迄今为止，获得在高温还原气氛下运行稳定的乙烷脱氢催化剂仍然是一个巨大的挑战。在这项研究中，我们制备了一种负载在 MgAl 2 O 4上的铁基催化剂，其铁物种原子分散，即使在 6 个反应-再生循环后也是如此。MgAl 2 O 4的片状形貌和尖晶石结构有利于Fe物种的高度分散。原位高角度环形暗场扫描透射电子显微镜和准原位 57 Fe穆斯堡尔谱证明了铁物质在乙烷脱氢反应过程中经历了还原、烧结和分离。相比之下，CO 2的引入导致缓慢失活，其中仅观察到孤立的Fe 3+物质部分还原为孤立的Fe 2+物质。通过简单的O 2处理即可恢复活性。目前的工作揭示了高效脱氢催化剂的设计。
更新日期：2023-08-08
中文翻译：
乙烷脱氢反应过程中 CO2 共进料对 MgAl2O4 上原子分散铁物种稳定性的影响
乙烷脱氢为页岩气的有效利用和生产乙烯提供了机会。迄今为止，获得在高温还原气氛下运行稳定的乙烷脱氢催化剂仍然是一个巨大的挑战。在这项研究中，我们制备了一种负载在 MgAl 2 O 4上的铁基催化剂，其铁物种原子分散，即使在 6 个反应-再生循环后也是如此。MgAl 2 O 4的片状形貌和尖晶石结构有利于Fe物种的高度分散。原位高角度环形暗场扫描透射电子显微镜和准原位 57 Fe穆斯堡尔谱证明了铁物质在乙烷脱氢反应过程中经历了还原、烧结和分离。相比之下，CO 2的引入导致缓慢失活，其中仅观察到孤立的Fe 3+物质部分还原为孤立的Fe 2+物质。通过简单的O 2处理即可恢复活性。目前的工作揭示了高效脱氢催化剂的设计。
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