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Molecular Reactions of O2 and CO2 on Ionically Conducting Catalyst
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-17 00:00:00 , DOI: 10.1021/acscatal.7b03467
Yi-Lin Huang 1 , Christopher Pellegrinelli 1 , Mann Sakbodin 1 , Eric D. Wachsman 1
Affiliation  

The presence of CO2, an unavoidable component in air and fuel environments, is known to cause severe performance degradation in oxide catalysts. Understanding the interactions between O2, CO2, and ion-conducting oxides is critical to developing energy-conversion devices. Here, surface reaction kinetics of Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) with the presence of both O2 and CO2 is determined using gas-phase isotope exchange. BSCF actively reacts with CO2, and the incorporation of oxygen from CO2 to the lattice of BSCF is directly observed as low as 50 °C. Above 200 °C, the reaction between CO2 and the BSCF surface dominates and is independent of the oxygen partial pressure. In addition, CO2 competes with O2 for binding to vacancy sites, forming surface intermediate species. Surprisingly, these surface intermediate species offer oxygen to exchange with oxygen in gaseous O2 and CO2, inhibiting the interactions between O2 and the solid surface. This work provides fundamental insight into functioning oxide catalysts, and the results can be applied to the design of improved oxide catalysts.

中文翻译:

O 2和CO 2在离子导电催化剂上的分子反应

众所周知,空气和燃料环境中不可避免的组分CO 2的存在会导致氧化物催化剂的性能严重下降。了解O 2,CO 2和离子导电氧化物之间的相互作用对于开发能量转换装置至关重要。在此,使用气相同位素交换确定在存在O 2和CO 2的情况下Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O3 (BSCF)的表面反应动力学。BSCF与CO 2积极反应,并吸收来自CO 2的氧气直接观察到BSCF晶格的温度低至50°C。高于200°C,CO 2和BSCF表面之间的反应占主导地位,并且与氧分压无关。此外,CO 2的竞争对手ø 2结合位点的空缺,形成表面中间物质。令人惊讶地,这些表面中间物质提供氧以与气态O 2和CO 2中的氧交换,从而抑制了O 2与固体表面之间的相互作用。这项工作为功能性氧化物催化剂提供了基本的见识,并且该结果可以应用于改进的氧化物催化剂的设计。
更新日期:2018-01-17
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