Towards full one-pass conversion of carbon dioxide to methanol and methanol-derived products
Towards full one-pass conversion of carbon dioxide to methanol and methanol-derived products
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DOI：
10.1016/j.jcat.2013.09.005
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发表时间：
2014-01-01
影响因子：
7.3
通讯作者：
Urakawa, Atsushi
中科院分区：
文献类型：
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作者：
Bansode, Atul;Urakawa, Atsushi
对全球变暖和碳循环不平衡的日益关注促使快速开发高效的CO2转化工艺。我们报告了一种非常有效的合成甲醇的方法，该方法通过在高压条件下（高达360 bar）在共沉淀Cu/ZnO/Al 2 O3催化剂上连续催化氢化CO2来进行。在优化的反应条件范围内，实现了出色的单程CO2转化率（>95%）和甲醇选择性（>98%）。在182，000 h（-1）的非常高的GHSV下，在商业甲醇合成催化剂上，该方法提供7.7 gmecai g h（-1），这是迄今为止报道的最高收率值，代价是降低的CO2转化率（65.8%）和甲醇选择性（77.3%）。采用Cu/ZnO/Al_2 O_3和H-ZSM-5催化剂组成的混合床，在CO_2转化率相当或更高的条件下，CO_2一步转化为二甲醚的选择性达到89%。此外，我们证明，从甲醇合成反应器中流出的甲醇，富含Hy和水，可以直接进料到含有H-ZSM-5催化剂的反应器中，用于选择性地生产烷烃（85%）或烯烃（42%），这取决于二级反应器的操作压力。(C)2013 Elsevier Inc. All rights reserved.
The rising concerns about global warming and imbalance in the carbon cycle urge rapid development of efficient CO2 conversion processes. We report an exceptionally productive process for the synthesis of methanol via continuous catalytic hydrogenation of CO2 under high-pressure conditions (up to 360 bar) over co-precipitated Cu/ZnO/Al2O3 catalysts. Outstanding one-pass CO2 conversion (>95%) and methanol selectivity (>98%) were achieved under an optimized range of reaction conditions. At a very high GHSV of 182,000 h(-1) over a commercial methanol synthesis catalyst, the process delivers 7.7 gmecai g h(-1), which is by far the highest yield value reported to date, at the expense of lowered CO2 conversion (65.8%) and methanol selectivity (77.3%). Using a mixed bed consisting of the Cu/ZnO/Al2O3 and H-ZSM-5 catalysts, one-step conversion of CO2 into dimethyl ether with remarkable selectivity (89%) was attained at the equivalent or higher CO2 conversion level. Furthermore, we demonstrate that the effluent stream of methanol, rich in Hy and water, from the methanol synthesis reactor can be directly fed to a reactor containing the H-ZSM-5 catalyst for selective production of alkane (85%) or alkene (42%), depending on the operating pressure of the secondary reactor. (C) 2013 Elsevier Inc. All rights reserved.