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Syngas production using CO2-rich residues: From ideal to real operating conditions
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-07-31 , DOI: 10.1016/j.jcou.2021.101661
Miriam González-Castaño 1 , Judith González-Arias 1, 2 , Marta Elena Sánchez 2 , Jorge Cara-Jiménez 2 , Harvey Arellano-García 1
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Employing a series of Cu-MnOx supported catalysts, this work investigates for the first time the impact on the RWGS reaction rate obtained under simulated residual CO2-rich feed streams, i.e., when CO and CH4 species are added to the reaction atmosphere. For this purpose, a simulated gaseous stream was prepared based on real biomass processing results. First, the series of catalysts was assessed under diluted ideal conditions (i.e., a mixture of only CO2 and H2 with N2 as dilutant). Here, the catalysts’ performance depended on both metal size and surface basic sites. Still, as the CO2 partial pressure was increased (varying the H2:CO2 ratio), the Cu metal dispersion seemed the catalyst feature governing RWGS reaction rate. Values of CO2 conversion from 50 to 60 % were registered for the different catalysts at a ratio H2:CO2 of 4. Then, under simulated residuals conditions and aside of thermodynamic limitations, the achievement of improved catalyst performances also depended on the catalysts’ reactivity towards the oxidation of CH4 fractions. For (X wt.%) Cu - (10 wt.%) MnOx/Al2O3 catalysts, 10 wt.% Cu was determined as the optimal Cu content. With this selected value, over the different analyzed supports (γ-Al2O3, (5 wt.%) SiO2-Al2O3, (40 wt.%) SiO2-Al2O3 and (20 wt.%) CeO2-Al2O3), the highest conversion rates with values of CO2 conversion of ca. 50 % at the higher temperature and optimal catalyst stabilities attained by the ceria supported catalyst (close to 95 % at most of the reaction temperatures) were ascribed to the optimal particle sizes and promoted CH4 activation processes.



中文翻译:

使用富含二氧化碳的残渣生产合成气:从理想到实际操作条件

采用一系列 Cu-MnO x负载催化剂,这项工作首次研究了在模拟的富含 CO 2 的残留进料流下获得的 RWGS 反应速率的影响,即当 CO 和 CH 4物种添加到反应气氛中时. 为此,基于真实的生物质加工结果制备了模拟气流。首先,在稀释的理想条件(即,仅CO 2和H 2的混合物,N 2作为稀释剂)下评估该系列催化剂。在这里,催化剂的性能取决于金属尺寸和表面碱性位点。尽管如此,随着 CO 2分压的增加(改变 H 2:CO 2比率),Cu 金属分散体似乎是控制 RWGS 反应速率的催化剂特征。在 H 2 :CO 2为 4的比率下,记录了不同催化剂的 CO 2转化率从 50% 到 60% 的值。然后,在模拟残留条件下,除了热力学限制外,提高催化剂性能的实现也取决于催化剂' 对 CH 4馏分氧化的反应性。对于(X wt.%) Cu - (10 wt.%) MnO x /Al 2 O 3催化剂,10 wt.% Cu被确定为最佳Cu含量。使用此选定值,在不同的分析载体 (γ-Al 2 O 3, (5 wt.%) SiO 2 -Al 2 O 3 , (40 wt.%) SiO 2 -Al 2 O 3和 (20 wt.%) CeO 2 -Al 2 O 3 ),转化率最高的 CO 2转化约。在较高温度下 50% 和由氧化铈负载的催化剂获得的最佳催化剂稳定性(在大多数反应温度下接近 95%)归因于最佳粒度并促进了 CH 4活化过程。

更新日期:2021-08-01
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