Identifying correlations in Fischer-Tropsch synthesis and CO2 hydrogenation over Fe-based ZSM-5 catalysts
Identifying correlations in Fischer-Tropsch synthesis and CO2 hydrogenation over Fe-based ZSM-5 catalysts
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Fe基ZSM-5催化剂上F-T合成和CO2加氢反应的相关性研究
DOI：
10.1016/j.jcou.2020.101290
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发表时间：
2020-10-01
影响因子：
7.7
通讯作者：
Porosoff, Marc D.
中科院分区：
文献类型：
--
作者：
Liu, Renjie;Ma, Zhiqiang;Porosoff, Marc D.
本文研究了Fe负载于ZSM-5（Si/Al = 50）的酸性（H）和钠（Na）型分子筛上进行费托合成（FTS）和CO2加氢反应的相关性。FTS反应器研究表明，由于Na增加了催化剂的表面碱性，烯烃的选择性从Fe/H-ZSM-5的11%增加到Fe/Na-ZSM-5的29.4%。反应器研究扩展到CO2加氢，其中逆水煤气变换是主要反应，Fe/Na-ZSM-5显示出增强的CO2吸附，并且反过来，与Fe/H-ZSM-5（类似于60%）相比，具有更高的CO选择性（类似于80%）。催化剂的特征在于通过各种分析技术，包括穆斯堡尔光谱，傅里叶变换红外（FTIR）光谱和程序升温脱附（TPD）的NH3和CO2的酸-碱性质与催化性能的关联。本研究的结果清楚地表明，FTS和CO2加氢的选择性可以通过用钠改性催化剂的酸碱性质而向所需产物衰减。这些结果是设计用于从CO和CO2合成轻质烯烃的高性能催化剂的重要一步。
Correlations in Fischer-Tropsch synthesis (FTS) and CO2 hydrogenation are investigated over Fe supported on the acidic (H) and sodium (Na) forms of ZSM-5 (Si/Al = 50). FTS reactor studies indicate the selectivity toward olefins increases from 11% over Fe/H-ZSM-5 to 29.4% over Fe/Na-ZSM-5 because of Na increasing the surface basicity of the catalyst. Reactor studies are extended to CO2 hydrogenation, where reverse water-gas shift is the dominant reaction, with Fe/Na-ZSM-5 displaying enhanced CO2 adsorption, and in turn, higher CO selectivity (similar to 80%) versus Fe/H-ZSM-5 (similar to 60%). The catalysts are characterized by a variety of analytical techniques including Mossbauer spectroscopy, Fourier transform infrared (FTIR) spectroscopy and temperature programmed desorption (TPD) of NH3 and CO2 to correlate acid-base properties with catalytic performance. The findings of this study clearly show the selectivity of FTS and CO2 hydrogenation can be attenuated toward the desired products by modifying the acid-base properties of the catalyst with sodium. These results are an important step toward designing high-performance catalysts for light olefin synthesis from CO and CO2.y