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Catalyst screening for the oxidative coupling of methane: from isothermal to adiabatic operation via microkinetic simulations
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020/01/30 , DOI: 10.1039/c9re00478e Laura Pirro 1, 2, 3, 4 , Pedro S. F. Mendes 1, 2, 3, 4 , Bart D. Vandegehuchte 4, 5, 6 , Guy B. Marin 1, 2, 3, 4 , Joris W. Thybaut 1, 2, 3, 4
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020/01/30 , DOI: 10.1039/c9re00478e Laura Pirro 1, 2, 3, 4 , Pedro S. F. Mendes 1, 2, 3, 4 , Bart D. Vandegehuchte 4, 5, 6 , Guy B. Marin 1, 2, 3, 4 , Joris W. Thybaut 1, 2, 3, 4
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A microkinetics-based study was performed on the relevance of conventional isothermal data for the selection of catalysts for oxidative coupling of methane (OCM) in adiabatic reactors. Catalyst performances from isothermal tests in oxygen-lean feeds (CH4/O2 ≥ 7) were found to reliably indicate the catalyst ranking for adiabatic operation, which features large methane excess for temperature control reasons. In such conditions, the concentration of surface oxygen was found to be significantly lower on the top-performing catalysts. This was attributed to the lower contribution of surface reactions, which is beneficial for C2+ selectivity at iso-conversion. However, these relevant isothermal data are scarce in literature because typically oxygen-rich (CH4/O2 < 5) reaction conditions are used to maximize the C2+ yield. Therefore the majority of lab-scale tests at isothermal conditions might have resulted in the rejection of catalysts that could perform reasonably well in adiabatic reactors. The insights gained via kinetic and statistical analysis were further elaborated to suggest experimental guidelines for future isothermal benchmarking of OCM catalysts in view of the industrially-relevant adiabatic operation.
中文翻译：
甲烷氧化偶联催化剂的筛选：通过微动力学模拟从等温到绝热操作
在常规等温数据与选择绝热反应器中甲烷氧化偶联（OCM）催化剂的相关性方面，进行了基于微动力学的研究。从等温试验的催化剂性能在贫氧进料（CH 4 / O 2，发现≥7）可靠地指示所述催化剂排名绝热操作，其特点大甲烷过量用于温度控制的原因。在这样的条件下，发现在性能最佳的催化剂上表面氧的浓度明显较低。这归因于表面反应的较低贡献，这有利于等转化时的C 2+选择性。但是，这些相关的等温数据在文献中很少，因为通常富含氧气（CH4 / O 2 <5）反应条件用于最大化C 2+产率。因此，大多数在等温条件下进行的实验室规模的测试可能导致拒绝了在绝热反应器中表现良好的催化剂。进一步阐述了通过动力学和统计分析获得的见解，从而鉴于工业相关的绝热操作，为将来的OCM催化剂等温基准化提供了实验指导。
更新日期：2020-03-03
中文翻译：
甲烷氧化偶联催化剂的筛选：通过微动力学模拟从等温到绝热操作
在常规等温数据与选择绝热反应器中甲烷氧化偶联（OCM）催化剂的相关性方面，进行了基于微动力学的研究。从等温试验的催化剂性能在贫氧进料（CH 4 / O 2，发现≥7）可靠地指示所述催化剂排名绝热操作，其特点大甲烷过量用于温度控制的原因。在这样的条件下，发现在性能最佳的催化剂上表面氧的浓度明显较低。这归因于表面反应的较低贡献，这有利于等转化时的C 2+选择性。但是，这些相关的等温数据在文献中很少，因为通常富含氧气（CH4 / O 2 <5）反应条件用于最大化C 2+产率。因此，大多数在等温条件下进行的实验室规模的测试可能导致拒绝了在绝热反应器中表现良好的催化剂。进一步阐述了通过动力学和统计分析获得的见解，从而鉴于工业相关的绝热操作，为将来的OCM催化剂等温基准化提供了实验指导。
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