渗氮和热处理对炭还原NO的活性影响及机理研究
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摘要
NO_x不仅是大气污染物的主要成分,而且会造成二次污染,已成为当前大气污染防治的主要对象。我国NO_x的工业源排放情况十分严重,这些排放源常集中分布在城市或者工业密集区域,其排放口低,NO_x浓度很高,其危害性和潜在危害性大,因此,工业高浓NO_x废气的治理具有重要意义。
目前用于治理工业高浓NO_x废气的技术各有优势,但也存在明显的不足,高效、经济的NO_x治理技术的开发已成为该领域的研究热点。活性炭在适宜的反应条件下可表现出良好的脱硝性能,与气态还原组分相比,其来源丰富、成本低廉、不会产生二次污染,在工业高浓NO_x废气治理领域有良好的应用前景。由于该过程是一个气-固相反应,所以活性炭的表面化学性质对NO_x的还原有重要影响,但有关此方面的研究较缺乏,还需要进行更多基础研究,为此工艺的工业化应用莫定基础。
本论文通过渗氮和热处理对活性炭和载铁活性炭进行了改性,借助元素分析、XRD、XPS、TPD-MS和TGA等手段,研究了渗氮和热处理对活性炭表面物化性质的影响规律,同时通过TPR和ISOR实验,考察了改性活性炭反应活性和选择性,并关联表征分析,探讨了渗氮和热处理对活性炭还原NO反应的影响机理及动力学。结果表明:
1、渗氮和热处理对活性炭表面化学性质的影响明显。当活性炭经氨气热处理1～4h后,表面氧含量显著降低,同时表面形成稳定的含氮官能团,而热处理主要降低了其表面氧含量。
2、氨气热处理渗氮的活性中心是炭表面的C-OH基团,渗入的氮原子大多位于石墨层结构的边缘,主要以N-5和N-6形态存在。Fe_2O_3的存在提高了活性炭的渗氮效果,C=O基团是载铁活性炭的渗氮活性中心。
3、在有氧条件下,活性炭的渗氮处理将其起始反应温度降低了约200℃,同时提高了活性炭的低温反应活性和选择性。表面含氮官能团可能作为催化活性中心促进了活性中间产物NO_2的生成,其可以提高活性炭的低温反应活性。与活性炭相比,渗氮活性炭还原NO反应的表观活化能降低了60-80%。
4、在有氧条件下,渗氮的载铁活性炭表现出优异的反应活性,其在500℃的NO_x转化率超过40%,这归因于活性炭表面Fe_2O_3和含氮官能团对C-NO反应的协同促进作用。渗氮后,载铁活性炭的反应选择性提高了40～60%,表观活化能降低了30-60%。
5、在无氧条件下,活性炭热处理降低了其还原NO的反应活性,且其反应活性随着热处理程度的加深而降低,这与炭表面C-OH数量的减少有直接关系,C-OH在C-NO反应中扮演了重要角色。在有氧条件下,热处理对活性炭反应活性的影响可以忽略。
NO_x is the major pollutant in the atmosphere,and it can also result in some secondary pollution,so it has been regarded as the main object in the treatment of air pollution.The pollution of NO_x from industrial sources is serious,and these sources usually locate in some cities and industrial areas,so the hazardness and potential hazardness is severe,therefore,it's very meaningful to harness the high concentration NO_x from industry.
At present,many technologies to deal with the high concentration NO_x have both advantages and disadvantages,so the development of the efficient and economical technology is an interesting subject in the field.Compared with the gaseous reducing agents,activated carbons can also show good performance in the reduction of NO_x. Moreover,they are cheap and free of secondary pollution besides abundant sources, which make them a well applicable perspective in the field of DeNOx.Because the reduction of NO by carbon is a heterogeneous reaction,the effect of surface chemistries on the reaction is very important,but there some few related studies,so it is necessary to do more basic research.
Some activated carbons were modified by nitrogen doping and heat treatment,and the regularity for change of the surface physicochemical characters was studied with kinds of measurement technologies such as elemental analyzer,XRD,XPS,TPD-MS, TGA and so on.At the same time,the reduction of NO with the modified carbons was investigated in a fixed-bed reactor when oxygen was both present and absent. Combined with the above analysis of the surface chemistries,the mechanisms for the reduction of NO with the modified carbons were studied in details.Results show that:
1.The effect of both nitrogen doping and heat treatment on the surface chemistries is significant.When the carbons had been annealed in ammonia for 1～4h,the surface oxygen content decreased greatly,while the surface nitrogen content increased by 1～4 times.The main change of the surface chemistries was the surface oxygen content by the heat treatment,and it deceased by 45%when the carbon had been heated at 800℃for 4h.
2.The active site for nitrogen doping by annealing in ammonia is C-OH,and most incorporated nitrogen atoms locate at the edges of graphene structures,especially in the form of N-6 and N-5.The existence of Fe_2O_3 particles can facilitate the nitrogen doping,and C=O is the active site for the nitrogen doping.
3.The reduction of NO with the carbon becomes noticeable at about 500℃in the presence of oxygen,but the reaction begins at about 300℃with the nitrogen-doped carbon,and the NO_x conversion is as high as 18%at 500℃.It may be attributed to the formation of NO_2 with the help of surface nitrogen species as catalytic centers. Compared with the pure carbon,both the reactivity and selectivity of the modified carbons increase greatly,and the apparent activation energy of the reduction of NO by the modified carbons decreases by 60～80%.
4.The carbon that is incorporated both nitrogen and Fe_2O_3 shows excellent activity for the reduction of NO in the presence of oxygen,and the NO_x conversion is higher than 40%at 500℃,which is due to the cooperative effect of Fe_2O_3 and the surface nitrogen species.Moreover the selectivity of modified carbon increases by 40～60%, and the apparent activation energy decreases by 30～60%.
5.When oxygen is absent,the heat treatment has a negative effect on the activity of the carbon,and the deeper heat treatment results in the lower activity,which is directly relevant to the decrease of the amount of C-OH which plays an important role in the reduction of NO with carbon.But the effect can be neglected in the presence of oxygen.
目前用于治理工业高浓NO_x废气的技术各有优势,但也存在明显的不足,高效、经济的NO_x治理技术的开发已成为该领域的研究热点。活性炭在适宜的反应条件下可表现出良好的脱硝性能,与气态还原组分相比,其来源丰富、成本低廉、不会产生二次污染,在工业高浓NO_x废气治理领域有良好的应用前景。由于该过程是一个气-固相反应,所以活性炭的表面化学性质对NO_x的还原有重要影响,但有关此方面的研究较缺乏,还需要进行更多基础研究,为此工艺的工业化应用莫定基础。
本论文通过渗氮和热处理对活性炭和载铁活性炭进行了改性,借助元素分析、XRD、XPS、TPD-MS和TGA等手段,研究了渗氮和热处理对活性炭表面物化性质的影响规律,同时通过TPR和ISOR实验,考察了改性活性炭反应活性和选择性,并关联表征分析,探讨了渗氮和热处理对活性炭还原NO反应的影响机理及动力学。结果表明:
1、渗氮和热处理对活性炭表面化学性质的影响明显。当活性炭经氨气热处理1～4h后,表面氧含量显著降低,同时表面形成稳定的含氮官能团,而热处理主要降低了其表面氧含量。
2、氨气热处理渗氮的活性中心是炭表面的C-OH基团,渗入的氮原子大多位于石墨层结构的边缘,主要以N-5和N-6形态存在。Fe_2O_3的存在提高了活性炭的渗氮效果,C=O基团是载铁活性炭的渗氮活性中心。
3、在有氧条件下,活性炭的渗氮处理将其起始反应温度降低了约200℃,同时提高了活性炭的低温反应活性和选择性。表面含氮官能团可能作为催化活性中心促进了活性中间产物NO_2的生成,其可以提高活性炭的低温反应活性。与活性炭相比,渗氮活性炭还原NO反应的表观活化能降低了60-80%。
4、在有氧条件下,渗氮的载铁活性炭表现出优异的反应活性,其在500℃的NO_x转化率超过40%,这归因于活性炭表面Fe_2O_3和含氮官能团对C-NO反应的协同促进作用。渗氮后,载铁活性炭的反应选择性提高了40～60%,表观活化能降低了30-60%。
5、在无氧条件下,活性炭热处理降低了其还原NO的反应活性,且其反应活性随着热处理程度的加深而降低,这与炭表面C-OH数量的减少有直接关系,C-OH在C-NO反应中扮演了重要角色。在有氧条件下,热处理对活性炭反应活性的影响可以忽略。
NO_x is the major pollutant in the atmosphere,and it can also result in some secondary pollution,so it has been regarded as the main object in the treatment of air pollution.The pollution of NO_x from industrial sources is serious,and these sources usually locate in some cities and industrial areas,so the hazardness and potential hazardness is severe,therefore,it's very meaningful to harness the high concentration NO_x from industry.
At present,many technologies to deal with the high concentration NO_x have both advantages and disadvantages,so the development of the efficient and economical technology is an interesting subject in the field.Compared with the gaseous reducing agents,activated carbons can also show good performance in the reduction of NO_x. Moreover,they are cheap and free of secondary pollution besides abundant sources, which make them a well applicable perspective in the field of DeNOx.Because the reduction of NO by carbon is a heterogeneous reaction,the effect of surface chemistries on the reaction is very important,but there some few related studies,so it is necessary to do more basic research.
Some activated carbons were modified by nitrogen doping and heat treatment,and the regularity for change of the surface physicochemical characters was studied with kinds of measurement technologies such as elemental analyzer,XRD,XPS,TPD-MS, TGA and so on.At the same time,the reduction of NO with the modified carbons was investigated in a fixed-bed reactor when oxygen was both present and absent. Combined with the above analysis of the surface chemistries,the mechanisms for the reduction of NO with the modified carbons were studied in details.Results show that:
1.The effect of both nitrogen doping and heat treatment on the surface chemistries is significant.When the carbons had been annealed in ammonia for 1～4h,the surface oxygen content decreased greatly,while the surface nitrogen content increased by 1～4 times.The main change of the surface chemistries was the surface oxygen content by the heat treatment,and it deceased by 45%when the carbon had been heated at 800℃for 4h.
2.The active site for nitrogen doping by annealing in ammonia is C-OH,and most incorporated nitrogen atoms locate at the edges of graphene structures,especially in the form of N-6 and N-5.The existence of Fe_2O_3 particles can facilitate the nitrogen doping,and C=O is the active site for the nitrogen doping.
3.The reduction of NO with the carbon becomes noticeable at about 500℃in the presence of oxygen,but the reaction begins at about 300℃with the nitrogen-doped carbon,and the NO_x conversion is as high as 18%at 500℃.It may be attributed to the formation of NO_2 with the help of surface nitrogen species as catalytic centers. Compared with the pure carbon,both the reactivity and selectivity of the modified carbons increase greatly,and the apparent activation energy of the reduction of NO by the modified carbons decreases by 60～80%.
4.The carbon that is incorporated both nitrogen and Fe_2O_3 shows excellent activity for the reduction of NO in the presence of oxygen,and the NO_x conversion is higher than 40%at 500℃,which is due to the cooperative effect of Fe_2O_3 and the surface nitrogen species.Moreover the selectivity of modified carbon increases by 40～60%, and the apparent activation energy decreases by 30～60%.
5.When oxygen is absent,the heat treatment has a negative effect on the activity of the carbon,and the deeper heat treatment results in the lower activity,which is directly relevant to the decrease of the amount of C-OH which plays an important role in the reduction of NO with carbon.But the effect can be neglected in the presence of oxygen.
引文
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