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Direct and selective hydrogenation of CO2 to ethylene and propene by bifunctional catalysts

机译：直接和选择性加氢的二氧化碳乙烯和丙烯的双功能催化剂

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摘要

Reduction of CO2 by H-2 produced from renewable electricity on a large scale would benefit both carbon recycling as well as H-2 storage and transport. Among the various CO2 hydrogenation reaction products, light olefins, such as ethylene and propylene, are very important intermediates in the chemical industry. However, very efficient catalytic systems that are able to drive CO2 hydrogenation reactions selectively to make olefins do not exist although the reactions are thermodynamically favorable. In this study, we demonstrated a selective hydrogenation process to directly convert CO2 to light olefins via a bifunctional catalyst composed of a methanol synthesis (In2O3/ZrO2) catalyst and a methanol-to-olefins (SAPO-34) catalyst. Under typical reaction conditions (e.g., 15 bar, 400 degrees C, and a space velocity of 12 L g(cat) (-1) h(-1)), light olefins (ethylene and propylene) with a selectivity of 80-90% in hydrocarbons can be obtained with a CO2 conversion of similar to 20%. To the best of our knowledge, this is the highest selectivity reported to date, which significantly surpasses the value obtained over conventional iron or cobalt CO2 Fischer-Tropsch synthesis catalysts (typically less than 50%). Moreover, our designed bifunctional catalyst shows good catalytic stability and can run for 50 h continuously without obvious activity decay. Our study provides an important contribution for CO2 conversion to value-added chemicals.
机译：减少2产生的二氧化碳来自可再生大规模的电力将会受益碳回收以及2存储交通工具。反应产品、轻烯烃等乙烯和丙烯,是非常重要的在化工中间体。能够非常有效的催化系统驱动二氧化碳加氢反应选择性使烯烃不存在虽然反应热力学是有利的。我们展示了一种选择性加氢过程直接将二氧化碳转换成轻烯烃通过双功能催化剂组成的甲醇催化剂和合成研究/氧化锆)methanol-to-olefins (SAPO-34)催化剂。典型的反应条件(如15条,40012摄氏度,空速L g (cat)(1) h(1)),轻烯烃(乙烯和丙烯选择性为80 - 90%碳氢化合物可以获得与二氧化碳类似于20%的转换。所知,这是最高的选择性报道,到目前为止,大大超过在传统的铁或获得的价值二氧化碳费托合成钴催化剂(通常低于50%)。双功能催化剂显示出了良好的催化能力稳定和连续运行50 h没有明显的放射性衰变。提供了二氧化碳的一个重要贡献转换增值的化学物质。

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