Direct Production of Lower Olefins from CO2 Conversion via Bifunctional Catalysis
Direct Production of Lower Olefins from CO2 Conversion via Bifunctional Catalysis
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双功能催化 CO2 转化直接生产低级烯烃
DOI：
10.1021/acscatal.7b02649
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发表时间：
2018-01-01
期刊：
影响因子：
12.9
通讯作者：
Sun, Yuhan
中科院分区：
文献类型：
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作者：
Gao, Peng;Dang, Shanshan;Sun, Yuhan
二氧化碳（CO2）直接转化为低烯烃(C-2(=)-C-4(=))，一般指乙烯、丙烯和丁烯，由于其在温室气体控制和化石燃料替代方面具有重要意义，作为一种可持续生产路线极具吸引力，但这种路线对烯烃的选择性往往较低。在这里，我们提出了一种双功能催化过程，在超过35%的CO2转化率下，C-2(=)-C-4（=）选择性高达80%，C-2-C-4选择性约为93%。这是通过一种由铟锆复合氧化物和SAPO-34沸石组成的双功能催化剂来实现的，它们分别负责CO2活化和选择性C-C偶联。我们证明了氧化物表面氧空位的精确控制和组分的集成方式对二氧化碳加氢直接生产低烯烃至关重要。在150小时内没有观察到明显的失活，表明有很好的工业应用潜力。
Direct conversion of carbon dioxide (CO2) into lower olefins (C-2(=)-C-4(=)), generally referring to ethylene, propylene, and butylene, is highly attractive as a sustainable production route for its great significance in greenhouse gas control and fossil fuel substitution, but such a route always tends to be low in selectivity toward olefins. Here we present a bifunctional catalysis process that offers C-2(=)-C-4(=) selectivity as high as 80% and C-2-C-4 selectivity around 93% at more than 35% CO2 conversion. This is achieved by a bifunctional catalyst composed of indium zirconium composite oxide and SAPO-34 zeolite, which is responsible for CO2 activation and selective C-C coupling, respectively. We demonstrate that both the precise control of oxygen vacancies on the oxide surface and the integration manner of the components are crucial in the direct production of lower olefins from CO2 hydrogenation. No obvious deactivation is observed over 150 h, indicating a promising potential for industrial application.