Iron-Potassium on Single-Walled Carbon Nanotubes as Efficient Catalyst for CO2 Hydrogenation to Heavy Olefins
Iron-Potassium on Single-Walled Carbon Nanotubes as Efficient Catalyst for CO2 Hydrogenation to Heavy Olefins
复制标题
单壁碳纳米管上的铁钾作为二氧化碳加氢制重烯烃的高效催化剂
DOI：
10.1021/acscatal.0c00810
复制
发表时间：
2020
期刊：
影响因子：
12.9
通讯作者：
Qiao Minghua
中科院分区：
文献类型：
--
作者：
Wang Shunwu;Wu Tijun;Lin Jun;Ji Yushan;Yan Shirun;Pei Yanting;Xie Songhai;Zong Baoning;Qiao Minghua
制备了单壁和多壁碳纳米管负载的铁钾催化剂FeK/SWNTs和FeK/MWNTs，并对其进行了表征和CO2加氢性能评价。在CO2加氢制烯烃反应中，FeK/SWNTs催化剂的选择性高于FeK/MWNTs催化剂，选择性分别为62.3%和52.4%。特别值得注意的是，FeK/SWNTs催化剂对重烯烃的选择性更高(C5+=选择性，39.8%)，而FeK/MWNTs催化剂对低碳烯烃的选择性更高(C2-C4=选择性，30.7%)。FeK/SWNTs催化剂对CO和CH4的选择性较低，烃的产率也较高，从而使重烯烃的产率达到27.6molCO2gFe-1s-1。具有较大曲率的单壁碳纳米管表面电子更加丰富，Haμ̈gg碳化物丰度较高，与低碳烯烃的相互作用较强，这可能是FeK/SWNTs催化剂在CO2加氢制重烯烃方面具有优越催化性能的原因。在120h的稳定性测试中，FeK/SWNTs催化剂的催化性能也有很小的变化，这表明SWNTs是一种很有前途的催化剂载体，可用于从温室气体二氧化碳中生产增值化学品。
The iron–potassium catalysts supported on single- and multiwalled carbon nanotubes, FeK/SWNTs and FeK/MWNTs, were fabricated, characterized, and evaluated in CO2hydrogenation. The FeK/SWNTs catalyst outperforms the FeK/MWNTs catalyst in selectivity during CO2hydrogenation to olefins with the selectivities being 62.3% and 52.4%, respectively. Of particular interest is that the FeK/SWNTs catalyst is more selective toward heavy olefins (C5+=selectivity, 39.8%), whereas the FeK/MWNTs catalyst is more selective to light olefins (C2–C4=selectivity, 30.7%). The FeK/SWNTs catalyst also affords much lower selectivities to undesired CO and CH4in addition to higher productivity of hydrocarbons, thus resulting in an unprecedentedly high productivity of heavy olefins of 27.6 μmolCO2gFe–1s–1. The more electron-enriched exterior of SWNTs with large curvature, higher abundance of Hägg carbide, and stronger interaction with light olefins may rationalize the superior catalytic behavior of the FeK/SWNTs catalyst in CO2hydrogenation to heavy olefins. The FeK/SWNTs catalyst also exhibited a minor change in catalytic performance in a 120 h stability test, highlighting SWNTs as a promising catalyst support for producing value-added chemicals from greenhouse gas CO2.