改性活性炭纤维（ACF）吸附气态汞的实验研究
摘要
燃煤造成的汞污染对生态环境具有极大的危害,随着人们环护意识的增强,汞污染问题逐渐得到重视。吸附剂喷射法是目前烟气汞排放控制的研究热点之一。在吸附剂研究方面,除活性炭外,还没有研究出可以推广使用的高效廉价吸附剂。因此,寻找有应用前景的高效烟气汞吸附剂,对于推动燃煤汞污染排放控制技术的发展将有重要的意义。
本文主要利用浸渍法制备9种改性活性炭纤维样品,气态汞吸附实验对比各样品的汞吸附容量,通过扫描电镜分析(Scanning Electron Microscopy, SEM)及X光电子能谱分析(X-ray Photoelectron Spectronscopy, XPS)深入研究影响吸附性能的表面结构特性和化学特性,揭示样品改性与气态汞吸附性能间的内在规律。主要工作和成果如下:
1.SEM分析发现,载银后Ag颗粒直径、载银量随AgNO3浓度的升高而增大;结晶点数量随浓度的升高而增多,且较多地分布在微孔边缘和交界处。XPS分析表明,载银后纤维表面出现Ag-O-C配位键,其中的Ag先一步与气态汞发生汞齐作用,极大地提升了载银吸附剂的吸附性能。
2.ACF-MnO2样品的SEM扫描图中基本无颗粒附着物,但元素能谱分析(Energy Dispersive Spectrometry, EDS)表明样品表面存在少量Mn元素;ACF-MoO_3表面附着着颗粒状物质。XPS分析表明,ACF-MoO_3样品表面存在MoO_3。
3.由XPS分析结果的S2p谱可知,ACF-MoS2样品表面存在3种化学状态的S即S2-、S和SO_4~(2-),结合Mo3d谱信息,可知硫化后ACF-MoS2表面存在MoS2物质,但硫化不完全,ACF-MoS2纤维表面还存在少量MoO_3。
4.吸附气态汞实验表明ACF-MoS2是9种改性样品中汞吸附能力最强的吸附剂。由XPS的分析结果可知,改性后样品表面负载了MoS2和少量单质S提高了吸附剂的汞吸附容量。此外,由于银汞齐具有良好的热脱附性,可以循环再生,因此在合适的改性条件下,载银活性炭纤维也是一种很有前景的高效吸附剂。
Mercury pollution caused by coal combustion has brought great harm to environment.With strengthening of people’s concept in environment protection, mercury pollution is becoming more of a concern. Currently, adsorbent injection has been a focal point of researches on mercury control in flue gases. And besides the activated carbon (AC), there have no adsorbents with high efficiency, low price and wide adaptability. Therefore, it is significant to find high efficient and broad prospect adsorbents.
In this paper, 9 kinds of modified ACF samples were obtained by impregnation and their adsoption capacities were determined with vapor mercury adsorption expriments. The interaction between sample modification and adsorption performance was revealed via futher study of surface structure properties and chemical characteries using scanning electron microscopy (SEM) and X-ray photoelectron spectronscopy (XPS). The main works and achievements were as follows:
1. Acorrding to SEM micrographs, silver particles were mainly distributed in the edge and at the junction of microporous of ACF surfaces, particle size and amount of active points on ACF increased with higher AgNO3 solution. XPS spectra results suggested that Ag-O-C formed on surface of ACFs during the modification, Ag of coordination bond took a lead to combine with mercury and then improved adsorption performance.
2. There were no particle deposits investigated on SEM image of ACF-MnO2, but the results of EDS indicated that a spot of Mn existed; while several particles adhered to ACF-MoO_3. And XPS spectra results indicated that MoO_3 was on surface of ACF-MoO_3.
3. It was clear from S2p of XPS, there were three chemical states of S, namely S2-, S and SO42-, on the surface of ACF-MoS2. Based on the information of Mo3d, sulphur treatment was not completely carried out and ACF-MoS2 contained both MoO_3 and MoS2.
4. The vapor mercury adsorption experiments indicated ACF-MoS2 was the best adsorbent among the 9 modified samples. After modification, MoS2 and a little S were impregnated into ACF-MoS2, which enhanced the adorsption. Because of favorable thermal desorption, silver supported ACF could be regenerated and was a promising and effective adsorbent with suitable modification.
本文主要利用浸渍法制备9种改性活性炭纤维样品,气态汞吸附实验对比各样品的汞吸附容量,通过扫描电镜分析(Scanning Electron Microscopy, SEM)及X光电子能谱分析(X-ray Photoelectron Spectronscopy, XPS)深入研究影响吸附性能的表面结构特性和化学特性,揭示样品改性与气态汞吸附性能间的内在规律。主要工作和成果如下:
1.SEM分析发现,载银后Ag颗粒直径、载银量随AgNO3浓度的升高而增大;结晶点数量随浓度的升高而增多,且较多地分布在微孔边缘和交界处。XPS分析表明,载银后纤维表面出现Ag-O-C配位键,其中的Ag先一步与气态汞发生汞齐作用,极大地提升了载银吸附剂的吸附性能。
2.ACF-MnO2样品的SEM扫描图中基本无颗粒附着物,但元素能谱分析(Energy Dispersive Spectrometry, EDS)表明样品表面存在少量Mn元素;ACF-MoO_3表面附着着颗粒状物质。XPS分析表明,ACF-MoO_3样品表面存在MoO_3。
3.由XPS分析结果的S2p谱可知,ACF-MoS2样品表面存在3种化学状态的S即S2-、S和SO_4~(2-),结合Mo3d谱信息,可知硫化后ACF-MoS2表面存在MoS2物质,但硫化不完全,ACF-MoS2纤维表面还存在少量MoO_3。
4.吸附气态汞实验表明ACF-MoS2是9种改性样品中汞吸附能力最强的吸附剂。由XPS的分析结果可知,改性后样品表面负载了MoS2和少量单质S提高了吸附剂的汞吸附容量。此外,由于银汞齐具有良好的热脱附性,可以循环再生,因此在合适的改性条件下,载银活性炭纤维也是一种很有前景的高效吸附剂。
Mercury pollution caused by coal combustion has brought great harm to environment.With strengthening of people’s concept in environment protection, mercury pollution is becoming more of a concern. Currently, adsorbent injection has been a focal point of researches on mercury control in flue gases. And besides the activated carbon (AC), there have no adsorbents with high efficiency, low price and wide adaptability. Therefore, it is significant to find high efficient and broad prospect adsorbents.
In this paper, 9 kinds of modified ACF samples were obtained by impregnation and their adsoption capacities were determined with vapor mercury adsorption expriments. The interaction between sample modification and adsorption performance was revealed via futher study of surface structure properties and chemical characteries using scanning electron microscopy (SEM) and X-ray photoelectron spectronscopy (XPS). The main works and achievements were as follows:
1. Acorrding to SEM micrographs, silver particles were mainly distributed in the edge and at the junction of microporous of ACF surfaces, particle size and amount of active points on ACF increased with higher AgNO3 solution. XPS spectra results suggested that Ag-O-C formed on surface of ACFs during the modification, Ag of coordination bond took a lead to combine with mercury and then improved adsorption performance.
2. There were no particle deposits investigated on SEM image of ACF-MnO2, but the results of EDS indicated that a spot of Mn existed; while several particles adhered to ACF-MoO_3. And XPS spectra results indicated that MoO_3 was on surface of ACF-MoO_3.
3. It was clear from S2p of XPS, there were three chemical states of S, namely S2-, S and SO42-, on the surface of ACF-MoS2. Based on the information of Mo3d, sulphur treatment was not completely carried out and ACF-MoS2 contained both MoO_3 and MoS2.
4. The vapor mercury adsorption experiments indicated ACF-MoS2 was the best adsorbent among the 9 modified samples. After modification, MoS2 and a little S were impregnated into ACF-MoS2, which enhanced the adorsption. Because of favorable thermal desorption, silver supported ACF could be regenerated and was a promising and effective adsorbent with suitable modification.
引文
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