Kinetics of Direct Olefin Synthesis from Syngas over Mixed Beds of Zn–Zr Oxides and SAPO-34,Industrial & Engineering Chemistry Research

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Kinetics of Direct Olefin Synthesis from Syngas over Mixed Beds of Zn–Zr Oxides and SAPO-34
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-09-24 , DOI: 10.1021/acs.iecr.1c03246
Joseph F. DeWilde ₁ , Christopher R. Ho ₁ , James Conner ₁ , Austin Smith ₁ , Alexey V. Kirilin ₂ , Andrzej Malek ₁ , Paul M. Witt ₁

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A packed bed containing a physical mixture of both Zn–Zr mixed oxide catalyst and SAPO-34 converts syngas directly into a mixture of C₂–C₅ olefins and paraffins. Specifically, the mixed oxide catalyst is responsible for intermediate oxygenate synthesis from syngas while the molecular sieve catalyzes olefin synthesis from the oxygenate intermediates. Kinetic measurements with cofed propylene over each catalyst independently confirm olefin hydrogenation activity over both components of the composite bed. The addition of either water or CO to the feed drops the activity of propylene hydrogenation over the Zn–Zr oxide. In sum, under reaction conditions of syngas feed and produced water, olefin hydrogenation predominantly occurs over the SAPO-34 catalyst, rather than over the catalyst responsible for hydrogenating CO into oxygenate intermediates. A developed kinetic model consistent with this conclusion describes measurements at differing feed compositions, temperatures, space velocities, and bed catalyst mixing ratios. Technoeconomic analysis of the process indicates that the olefin-to-paraffin ratio is a key performance metric for commercial scale syngas conversion and highlights the importance of considering olefin hydrogenation rates over the molecular sieve component.

中文翻译：

Zn-Zr 氧化物和 SAPO-34 混合床合成气直接合成烯烃的动力学

包含 Zn-Zr 混合氧化物催化剂和 SAPO-34 的物理混合物的填充床将合成气直接转化为 C ₂ -C ₅的混合物烯烃和石蜡。具体而言，混合氧化物催化剂负责从合成气合成中间体含氧化合物，而分子筛催化从含氧化合物中间体合成烯烃。用共进料丙烯在每种催化剂上的动力学测量独立地证实了复合床的两种组分上的烯烃加氢活性。向进料中添加水或 CO 会降低丙烯加氢活性超过 Zn-Zr 氧化物。总之，在合成气进料和采出水的反应条件下，烯烃加氢主要发生在 SAPO-34 催化剂上，而不是在负责将 CO 加氢成含氧化合物中间体的催化剂上发生。与该结论一致的开发动力学模型描述了在不同进料成分、温度、空间速度、和床催化剂混合比。该工艺的技术经济分析表明，烯烃与链烷烃的比率是商业规模合成气转化的关键性能指标，并强调了考虑分子筛组分上烯烃加氢速率的重要性。

更新日期：2021-10-06

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