Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted ...Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted with both potassium (K) and manganese (Mn) showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity (GHSV) of 3.1 L-(g·h)-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction (XRD), temperature-programmed reduction (TPR) with molecular hydrogen (H2), and in situ X-ray absorption near-edge structure (XANES) analysis. The Mn pro- moter stabilized wtistite (FeO) as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia (NH_3) decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.展开更多
基金supported by the Synchrotron Light Research Institute(Public Organization)Thailand(GS-54-D01)+7 种基金the Commission on Higher EducationMinistry of EducationThailandperformed under the project"Sustainable Chemical Synthesis(Sus Chem Sys)"which is co-financed by the European Regional Development Fund(ERDF)the state of North Rhine-WestphaliaGermanyunder the Operational Programme"Regional Competitiveness and Employment"2007–2013
文摘Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted with both potassium (K) and manganese (Mn) showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity (GHSV) of 3.1 L-(g·h)-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction (XRD), temperature-programmed reduction (TPR) with molecular hydrogen (H2), and in situ X-ray absorption near-edge structure (XANES) analysis. The Mn pro- moter stabilized wtistite (FeO) as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia (NH_3) decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.