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红壤吸附硫化氢的光谱研究

Spectroscopic study on sorption of hydrogen sulfide by means of red soil.

作者信息

Ko T H, Chu H

机构信息

Department of Environmental Engineering, National Cheng Kung University, Tainan City 70101, Taiwan.

出版信息

Spectrochim Acta A Mol Biomol Spectrosc. 2005 Jul;61(9):2253-9. doi: 10.1016/j.saa.2004.09.016. Epub 2004 Dec 18.

Abstract

This paper reports the results of the characterization of red soils in relation to the sorption of H2S from coal gas at 500 degrees C by spectroscopic techniques in order to provide more information on red soils' structural change both before and after reaction. In addition, by-products analysis has also been studied using Fourier transform infrared (FTIR) spectroscopy. Before and after the experiments the red soils were characterized with X-ray powder diffraction (XRPD), energy dispersion spectrum (EDS), X-ray photoelectron spectroscopy (XPS) and FTIR spectroscopy. XRPD results indicate that iron oxide species disappear from the original to reacted red soil. EDS analysis shows that a significant amount of sulfur is present in the reacted red soil, which is in agreement with the results of the elemental analysis and the calculated value based on breakthrough curve. XPS regression fitting results further indicate that sulfur retention may be associated with the iron oxides. S 2p XPS fittings point out that the major sulfur species present in the reacted red soil are composed of S(-2), elemental sulfur, polysulfide, sulfite and sulfate. Additionally, the binding energy of iron shifts to a lower position for the reacted red soil, which indicates that iron oxides in the original red soil have been converted into iron sulfide. Appreciable amounts of the by-products CO2, SO2 and COS are detected by on-line FTIR spectroscopy during the initial and later stages of the sorption process. The formation of CO2 is related to the water-shift reaction, and SO2 is probably attributable to the reaction of organic matters and H2S. The concentration of COS is quantified by GC/FPD and found it to be about 350 ppm, which is close to the equilibrium concentration of the reaction of inlet CO and H2S at a temperature of 500 degrees C.

摘要

本文报道了通过光谱技术对红壤在500℃下对煤气中H₂S吸附特性的表征结果,以便提供更多关于红壤反应前后结构变化的信息。此外,还利用傅里叶变换红外(FTIR)光谱对副产物进行了分析。在实验前后,用X射线粉末衍射(XRPD)、能量色散谱(EDS)、X射线光电子能谱(XPS)和FTIR光谱对红壤进行了表征。XRPD结果表明,从原始红壤到反应后的红壤,氧化铁物种消失。EDS分析表明,反应后的红壤中存在大量硫,这与元素分析结果和基于穿透曲线的计算值一致。XPS回归拟合结果进一步表明,硫的保留可能与氧化铁有关。S 2p XPS拟合指出,反应后的红壤中存在的主要硫物种由S(-2)、元素硫、多硫化物、亚硫酸盐和硫酸盐组成。此外,反应后的红壤中铁的结合能向较低位置移动,这表明原始红壤中的氧化铁已转化为硫化铁。在吸附过程的初始和后期阶段,通过在线FTIR光谱检测到了可观量的副产物CO₂、SO₂和COS。CO₂的形成与水煤气变换反应有关,SO₂可能归因于有机物与H₂S的反应。COS的浓度通过气相色谱/火焰光度检测器(GC/FPD)进行定量,发现其约为350 ppm,这与500℃下入口CO与H₂S反应的平衡浓度接近。

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