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CO2 Hydrogenation to Higher Alcohols over K-Promoted Bimetallic Fe–In Catalysts on a Ce–ZrO2 Support
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-04-29 , DOI: 10.1021/acssuschemeng.0c08760 Xiaoying Xi 1 , Feng Zeng 2 , Heng Zhang 3 , Xiaofeng Wu 4, 5 , Jie Ren 2 , Timo Bisswanger 6 , Christoph Stampfer 6 , Jan P. Hofmann 4, 5 , Regina Palkovits 2 , Hero J. Heeres 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-04-29 , DOI: 10.1021/acssuschemeng.0c08760 Xiaoying Xi 1 , Feng Zeng 2 , Heng Zhang 3 , Xiaofeng Wu 4, 5 , Jie Ren 2 , Timo Bisswanger 6 , Christoph Stampfer 6 , Jan P. Hofmann 4, 5 , Regina Palkovits 2 , Hero J. Heeres 1
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Novel K-promoted bimetallic Fe- and In-based catalysts on a Ce–ZrO2 support were prepared and tested for higher alcohol synthesis from CO2 and hydrogen. The FeIn/Ce–ZrO2 precursors with different Fe contents were characterized in detail, and well-dispersed Fe2O3 and In2O3 phases with oxygen vacancies were observed. The catalysts were tested in a continuous setup at extended times on stream (up to 100 h) at 300 °C, 10 MPa, a gas hourly space velocity of 4500 mL g–1 h–1, and a H2/CO2 ratio of 3. The effect of K loading, the pretreatment atmosphere, Fe/(Fe + In) molar ratios, and calcination temperature on CO2 conversion and product selectivity were studied. Best performance with a CO2 conversion of 29.6% and a higher alcohol selectivity of 28.7%, together with good stability, was obtained over a K-0.82-FeIn/Ce–ZrO2_900 catalyst after activation under a CO atmosphere. These findings were rationalized by considering the effects of the individual catalyst components (K, Fe, and In) on catalyst performance. Surprisingly, the presence of calcined SiC, used as a diluent in the packed bed reactor, was shown to have a positive effect on catalyst performance and as such also is catalytically active. The best performance in terms of higher alcohol yield (8.5%) obtained in this work ranks in the top three of reports on CO2 hydrogenation to higher alcohols in a continuous setup. Moreover, light olefins with 20.3% selectivity (6.0% yield) were coproduced over the optimized catalyst, which has a positive effect on the economic potential of the catalysts.
中文翻译：
Ce-ZrO 2载体上K促进双金属Fe-催化CO 2加氢成高级醇
制备了在Ce–ZrO 2载体上的新型K促进的双金属Fe和In基催化剂，并测试了由CO 2和氢合成高级醇的能力。详细描述了具有不同Fe含量的FeIn / Ce-ZrO 2前驱体，并观察到分散良好的Fe 2 O 3和In 2 O 3相具有氧空位。在连续设置下，在300°C，10 MPa，4500 mL g –1 h –1的气体时空速度和H 2 / CO 2的气态时空条件下（最长100 h）对催化剂进行了测试。研究了K负载，预处理气氛，Fe /（Fe + In）摩尔比和煅烧温度对CO 2转化率和产物选择性的影响。在K-0.82-FeIn / Ce–ZrO 2上获得了最佳性能，其中CO 2转化率为29.6％，酒精选择性更高，为28.7％，而且稳定性好。_900在CO气氛下活化后的催化剂。通过考虑各个催化剂组分（K，Fe和In）对催化剂性能的影响，可以合理化这些发现。出乎意料的是，已证明在填充床反应器中用作稀释剂的煅烧SiC的存在对催化剂性能具有积极影响，因此也具有催化活性。在这项工作中获得的最高酒精产率（8.5％）方面的最佳性能在连续设置中将CO 2加氢为高级酒精的报告中名列前三位。此外，在优化的催化剂上联产了具有20.3％选择性（6.0％收率）的轻质烯烃，这对催化剂的经济潜力产生了积极影响。
更新日期：2021-05-10
中文翻译：
Ce-ZrO 2载体上K促进双金属Fe-催化CO 2加氢成高级醇
制备了在Ce–ZrO 2载体上的新型K促进的双金属Fe和In基催化剂，并测试了由CO 2和氢合成高级醇的能力。详细描述了具有不同Fe含量的FeIn / Ce-ZrO 2前驱体，并观察到分散良好的Fe 2 O 3和In 2 O 3相具有氧空位。在连续设置下，在300°C，10 MPa，4500 mL g –1 h –1的气体时空速度和H 2 / CO 2的气态时空条件下（最长100 h）对催化剂进行了测试。研究了K负载，预处理气氛，Fe /（Fe + In）摩尔比和煅烧温度对CO 2转化率和产物选择性的影响。在K-0.82-FeIn / Ce–ZrO 2上获得了最佳性能，其中CO 2转化率为29.6％，酒精选择性更高，为28.7％，而且稳定性好。_900在CO气氛下活化后的催化剂。通过考虑各个催化剂组分（K，Fe和In）对催化剂性能的影响，可以合理化这些发现。出乎意料的是，已证明在填充床反应器中用作稀释剂的煅烧SiC的存在对催化剂性能具有积极影响，因此也具有催化活性。在这项工作中获得的最高酒精产率（8.5％）方面的最佳性能在连续设置中将CO 2加氢为高级酒精的报告中名列前三位。此外，在优化的催化剂上联产了具有20.3％选择性（6.0％收率）的轻质烯烃，这对催化剂的经济潜力产生了积极影响。
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