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高炉煤气中H2S在羟基氧化铁上的吸附氧化机理研究

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采用沉淀法制备了羟基氧化铁(α-FeOOH)吸附剂,利用固定床-气相色谱联用平台测试了其对H2S的吸附容量,发现其硫容达到了 63。8 mg/g,测试了 O2和H2O对硫容的影响,发现二者均存在最佳浓度,在选定条件下O2和H2O最佳浓度分别为0。3vol%和3vol%。采用XRD,XPS,TG和CO2-TPD等表征了吸附剂的理化性质及含硫组分的赋存形态,发现α-FeOOH吸附H2S后硫物种主要为硫单质和硫酸盐(SO42-)。通过预吸附氧气的方式分析了O2在反应中的作用,吸附态的氧促进硫单质形成,气态的O2存在会增加SO42-的比例。通过原位漫反射红外光谱测试了H2S吸附的中间产物,H2S在α-FeOOH表面吸附与晶格氧或羟基结合生成HS-,HS-被Fe3+氧化发生电子转移生成硫单质或者被O2氧化生成SO42-。本工作为吸附剂优化制备及高炉煤气净化技术应用提供了理论依据。
Study on adsorption and oxidation mechanisms of H2S in blast furnace gas on hydroxyl iron oxide
Precipitation method was used to prepare hydroxylated iron oxide(α-FeOOH)adsorbent to test its adsorption capacity for H2S using a fixed bed gas chromatography platform in this work.It was found that its sulfur capacity reached 63.8 mg/g,and the effects of O2 and H2O atmospheres on sulfur capacity were tested.It was found that there were optimal concentrations for O2 and H2O under the selected conditions,being 0.3vol%and 3vol%,respectively.The physicochemical properties of adsorbents and the occurrence forms of sulfur-containing components were characterized by XRD,XPS,TG,and CO2-TPD.It was found that the main sulfur-containing species were elemental sulfur and sulfate(SO42-)after α-FeOOH adsorbed H2S.The role of O2 in the reaction was analyzed by pre-adsorbing oxygen test.The adsorbed oxygen promoted the formation of sulfur elemental,while the presence of gaseous O2 increased the proportion of SO42-.In situ diffuse reflectance infrared spectroscopy showed the intermediate products adsorbed by H2S.H2S combined with the lattice oxygen or hydroxyl groups on α-FeOOH surface to generate HS-,and then HS-was further oxidized by Fe3+with electron transfer to generate elemental sulfur,or HS-was oxidized by O2 to generate SO42-.This work provides a theoretical basis for the optimization of adsorbent preparation and the application of blast furnace gas purification technology.

blast furnace gashydroxyl iron oxidehydrogen sulfideadsorption-oxidationsulfur capacity

刘旭东、李玉然、彭书雯、刘利、徐文青、朱廷钰

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华北理工大学化学工程学院,河北省环境光电催化材料重点实验室,河北唐山 063200

中国科学院过程工程研究所,中国科学院绿色过程制造创新研究院,北京 100190

高炉煤气 羟基氧化铁 硫化氢 吸附氧化 硫容

2024

过程工程学报
中国科学院过程工程研究所

过程工程学报

CSTPCD北大核心
影响因子:0.526
ISSN:1009-606X
年,卷(期):2024.24(12)