Oxidative Coupling of Methane over Hybrid Membrane/Catalyst Active Centers: Chemical Requirements for Prolonged Lifetime,ACS Energy Letters

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Oxidative Coupling of Methane over Hybrid Membrane/Catalyst Active Centers: Chemical Requirements for Prolonged Lifetime
ACS Energy Letters ( IF 19.3 ) Pub Date : 2019-06-03 00:00:00 , DOI: 10.1021/acsenergylett.9b01075
Valentina Omoze Igenegbai _{1,

2} , Rawan Almallahi _{1,

2} , Randall J. Meyer ₃ , Suljo Linic _{1,

2}

Affiliation

Solid oxide membrane/catalyst hybrid systems have been proposed as a promising platform for selective oxidative coupling of methane to form higher value C₂₊ products. In these hybrid systems, the membrane controls the local chemical potential of reacting oxygen atoms while the catalyst allows for selective reaction of these oxygen atoms with methane to form the desired C₂ products. One critical challenge with these systems is that due to relatively low local O₂/CH₄ ratios, they can promote carbon-induced catalyst deactivation. Herein, we demonstrate that a BaCe_0.8Gd_0.2O_3-δ based membrane/catalyst system can achieve excellent carbon resistance at low O₂/CH₄ ratios, and high and stable selectivity (over 80%) to C₂₊ products (ethane, ethylene, propane, and propylene). Our analysis of the system suggests that its high carbon resistance is due to its relatively high oxygen storage/release capacity which suppresses carbon deposition in the system.

中文翻译：

混合膜/催化剂活性中心上甲烷的氧化偶联：延长寿命的化学要求

固体氧化物膜/催化剂混合系统已经被提出作为甲烷选择性氧化偶联以形成更高价值的C ₂₊产物的有前途的平台。在这些混合系统中，膜控制着氧原子反应的局部化学势，而催化剂则允许这些氧原子与甲烷选择性反应以形成所需的C ₂产物。这些系统的一个关键挑战是由于相对较低的局部O ₂ / CH ₄比，它们可以促进碳诱导的催化剂失活。在本文中，我们证明了基于BaCe _0.8 Gd _0.2 O3 _-δ的膜/催化剂体系可以在低O下获得出色的耐碳性₂ / CH ₄比率，以及对C ₂₊产物（乙烷，乙烯，丙烷和丙烯）的高且稳定的选择性（超过80％）。我们对系统的分析表明，其较高的耐碳性是由于其较高的氧气存储/释放能力，抑制了系统中的碳沉积。

更新日期：2019-06-03

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