生物还原耦合化学吸收处理烟气中NO_x的关键因素及作用机制
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摘要
随着国民经济的发展,氮氧化物(NOx)的排放量持续增加,NOx造成的污染问题日益严重,并受到越来越多的关注。现有的烟气脱硝技术尚存在投资运行费用高、产生二次污染或者处理效率低等缺陷,为此,研究和开发具有处理效果好、投资及运行费用低、无二次污染等优点的新型烟气脱硝技术已经成为亟待解决的重大课题。
化学吸收-生物还原技术(CABR)处理烟气中NOx具有处理效果好、投资运行成本低等特点,因此在烟气脱硝领域具有广阔的应用前景。CABR技术的研发主要基于三方面：1)络合吸收剂选择和再生；2)络合态NO还原效率的提高；3)反应装置和工艺体系的研究。本文研究了CABR体系中一些关键因素如碳源的消耗及利用情况,氮元素在体系中的转化途径,并分析了该系统中各反应过程的限制性因素和生物膜中菌群结构分布特征,最后得到了最适合本系统的络合吸收体系。论文取得以下一些有价值的结果：
在化学吸收-生物还原技术中,采用葡萄糖作为碳源。Fe(Ⅲ)EDTA的还原过程需要足够的碳源来保证。葡萄糖代谢产物研究发现铁还原反应和络合态NO还原反应均受到乙酸积累的抑制。碳元素的平衡分析显示：典型的试验条件(670mg·m3NO,0-10%O2)下,化学吸收-生物还原体系中经过约240h的运行,超过一半的碳以气体的形式排出,生物相和液相中分别有19%和17%碳的积累。液相中的碳主要以VFA(乙酸)的形式存在,尾气中的碳主要以CO2的形式存在,且在低O2浓度条件下尾气中有少量的CH4生成。
化学吸收-生物还原体系中经过约90h的运行后,约66%的氮以气体的形式排出,生物相和液相中分别有18%和4%的氮的积累。液相中的氮主要以NO3-的形式存在,尾气中的氮主要以N2的形式存在,且尾气中没有发现N20的存在,只检测出少量的氮以N02的形式存在。有约5%的氮元素以其它形式存在或为试验误差。
在吸收-还原双塔中对生物还原耦合化学吸收净化烟气中NOx体系的过程反应速率分别进行研究。实验结果表明,Fe(Ⅱ)EDTA-NO生物还原反应速率>Fe(Ⅱ)EDTA氧化反应速率>Fe(Ⅲ)生物还原反应速率>NO络合吸收反应速率,在本系统中NO络合吸收反应和Fe(II)EDTA氧化反应是影响生物反应器高效脱除NO的限制性因素。
利用PCR-DGGE技术对生物填料塔稳态运行期间不同填料层微生物群落结构进行了初步分析。结果表明：生物填料塔内还原络合态NO的菌株主要属于假单胞菌(Pseudomonas sp.)。在整个O2浓度负荷提高的过程中,Escherichia coli在CABR系统中占据绝对的优势地位。
对稳定运行条件下不同吸收体系进行研究,考察模拟烟气中NO、O2、SO2浓度、气体流量、吸收液流量等参数对NO去除效率影响,通过处理效果等方面的比较获得了最优的络合吸收体系。实验结果表明：Fe(II)EDTA/Fe(II)Cit的混合配基体系具有最佳的技术参数。
With the development of the national economy and the increasing emission amount of NOx, the pollution caused by NOx becomes more serious and receive increasing attention of more people. Current technologies for NOx removal from flue gas have associated with some problems, such as high cost on investment and operation, producing secondary pollutant and low removal efficiency. So, to exploit a new technology which has advantages of low cost environment-friendly and high efficiency for NOX removal from flue gas is becoming an extremely urgent issue, presently.
A chemical absorption-biological reduction integrated approach is employed to achieve the removal of nitrogen monoxide (NO) from the simulated flue gas with the advantages of low cost, completely reduction of NO and high removal efficiency. The development of the integrated technologies includes two aspects:1) complex absorbent regeneration;2) NO bioreactor process control. In this dissertation, the key factors and mechanism of Fe(II)EDTA-NO reduction was investigated; the effects of carbon source, nitrogen cycle on this system were discussed; the feasibility of biological packed column with the integrated process was studied; through the analysis of biological reduction rates and NO absporption rates of NO process, the kinetic model was established. The main original conclusions of this dissertation are:
Glucose is suitable for the heterotrophic bacteria as the carbon source and electron donor to remove NO from simulated flue gas by the integrated chemical absorption-biological reduction system. In the range of0-10%oxygen concentration, the reactor can achieve long-term stable operation, and the removal efficiency of NO can be maintained above86%. The reduction of Fe(Ⅲ)EDTA mainly depends on the carbon source supplied. The studies on carbon source metabolites showed that the concentration of the accumulative acid determines whether the reduction of NO and Fe (Ⅲ) EDTA was inhibited. However, long-term stable operation of bioreactor could be achieved when there is acetic acid accumulation under aerobic conditions. The distribution of the carbon source degradation was also examined here with17%existed in the form of VFA, while50%total carbon source was consumed in the form of CO2. In addition, it was also found that glucose added into bioreactor within a certain range of oxygen concentrations will not be accumulated in the reactor, which keeps the operation stable.
After a run of93hours operation by chemical absorption-biological reduction integrated approach, about66%of the nitrogen discharged in the form of N2. The accumulation of nitrogen in the biological and liquid phases was18%and4%, respectively. The nitrogen in the liquid phase is mainly present in the form of NO3-, and there is no N2O presence of in the exhaust gas. Only a small amount of nitrogen present in the form of NO2and CH4. About5%of the nitrogen is in the form of other types or experimental error.
The reaction rate of NO absorption capacity by ferrous EDTA (Fe(II)EDTA) solution and reduction by microorganism were studied in an scrubber-bioreactor system.The results show that the order of the four reaction rates in reactor is as follow: Fe(II)EDTA-NO reduction rate> Fe(II)EDTA oxidation rate>Fe(III)EDTA reduction rate> NO absorption rate,so the NO absorption process and Fe(III)EDTA reduction are key steps for NO removal efficiency in this integrated system.
The microbial community structure in the biological packed tower was analyses with the PCR-DGGE technology. The microbial species at the top of the tower was least due to water erosion, while the bottom layer had the largest micro-organisms and less species. The similarity of microbial community structure increased with the increase height of packed bed. The preliminary analysis results indicated that the microorganisms in the biofilm belonged to β-Proteobacterium and Pseudomonas. The denitrifier was dominanted in the biofilm.
Investigate the influence on the NO removal efficiency of some elements such as the concentration of O2, NO, SO2, flow rate of inlet gas and absorbents. that the result of the influence on NO removal efficiency of the concentration of O2, NO, SO2, flow rate of inlet gas and absorbents was obtained. The results showed that the Fe(II)EDTA /Fe(Ⅱ)Cit mixed system has the best technical parameters and economic benefits.
化学吸收-生物还原技术(CABR)处理烟气中NOx具有处理效果好、投资运行成本低等特点,因此在烟气脱硝领域具有广阔的应用前景。CABR技术的研发主要基于三方面：1)络合吸收剂选择和再生；2)络合态NO还原效率的提高；3)反应装置和工艺体系的研究。本文研究了CABR体系中一些关键因素如碳源的消耗及利用情况,氮元素在体系中的转化途径,并分析了该系统中各反应过程的限制性因素和生物膜中菌群结构分布特征,最后得到了最适合本系统的络合吸收体系。论文取得以下一些有价值的结果：
在化学吸收-生物还原技术中,采用葡萄糖作为碳源。Fe(Ⅲ)EDTA的还原过程需要足够的碳源来保证。葡萄糖代谢产物研究发现铁还原反应和络合态NO还原反应均受到乙酸积累的抑制。碳元素的平衡分析显示：典型的试验条件(670mg·m3NO,0-10%O2)下,化学吸收-生物还原体系中经过约240h的运行,超过一半的碳以气体的形式排出,生物相和液相中分别有19%和17%碳的积累。液相中的碳主要以VFA(乙酸)的形式存在,尾气中的碳主要以CO2的形式存在,且在低O2浓度条件下尾气中有少量的CH4生成。
化学吸收-生物还原体系中经过约90h的运行后,约66%的氮以气体的形式排出,生物相和液相中分别有18%和4%的氮的积累。液相中的氮主要以NO3-的形式存在,尾气中的氮主要以N2的形式存在,且尾气中没有发现N20的存在,只检测出少量的氮以N02的形式存在。有约5%的氮元素以其它形式存在或为试验误差。
在吸收-还原双塔中对生物还原耦合化学吸收净化烟气中NOx体系的过程反应速率分别进行研究。实验结果表明,Fe(Ⅱ)EDTA-NO生物还原反应速率>Fe(Ⅱ)EDTA氧化反应速率>Fe(Ⅲ)生物还原反应速率>NO络合吸收反应速率,在本系统中NO络合吸收反应和Fe(II)EDTA氧化反应是影响生物反应器高效脱除NO的限制性因素。
利用PCR-DGGE技术对生物填料塔稳态运行期间不同填料层微生物群落结构进行了初步分析。结果表明：生物填料塔内还原络合态NO的菌株主要属于假单胞菌(Pseudomonas sp.)。在整个O2浓度负荷提高的过程中,Escherichia coli在CABR系统中占据绝对的优势地位。
对稳定运行条件下不同吸收体系进行研究,考察模拟烟气中NO、O2、SO2浓度、气体流量、吸收液流量等参数对NO去除效率影响,通过处理效果等方面的比较获得了最优的络合吸收体系。实验结果表明：Fe(II)EDTA/Fe(II)Cit的混合配基体系具有最佳的技术参数。
With the development of the national economy and the increasing emission amount of NOx, the pollution caused by NOx becomes more serious and receive increasing attention of more people. Current technologies for NOx removal from flue gas have associated with some problems, such as high cost on investment and operation, producing secondary pollutant and low removal efficiency. So, to exploit a new technology which has advantages of low cost environment-friendly and high efficiency for NOX removal from flue gas is becoming an extremely urgent issue, presently.
A chemical absorption-biological reduction integrated approach is employed to achieve the removal of nitrogen monoxide (NO) from the simulated flue gas with the advantages of low cost, completely reduction of NO and high removal efficiency. The development of the integrated technologies includes two aspects:1) complex absorbent regeneration;2) NO bioreactor process control. In this dissertation, the key factors and mechanism of Fe(II)EDTA-NO reduction was investigated; the effects of carbon source, nitrogen cycle on this system were discussed; the feasibility of biological packed column with the integrated process was studied; through the analysis of biological reduction rates and NO absporption rates of NO process, the kinetic model was established. The main original conclusions of this dissertation are:
Glucose is suitable for the heterotrophic bacteria as the carbon source and electron donor to remove NO from simulated flue gas by the integrated chemical absorption-biological reduction system. In the range of0-10%oxygen concentration, the reactor can achieve long-term stable operation, and the removal efficiency of NO can be maintained above86%. The reduction of Fe(Ⅲ)EDTA mainly depends on the carbon source supplied. The studies on carbon source metabolites showed that the concentration of the accumulative acid determines whether the reduction of NO and Fe (Ⅲ) EDTA was inhibited. However, long-term stable operation of bioreactor could be achieved when there is acetic acid accumulation under aerobic conditions. The distribution of the carbon source degradation was also examined here with17%existed in the form of VFA, while50%total carbon source was consumed in the form of CO2. In addition, it was also found that glucose added into bioreactor within a certain range of oxygen concentrations will not be accumulated in the reactor, which keeps the operation stable.
After a run of93hours operation by chemical absorption-biological reduction integrated approach, about66%of the nitrogen discharged in the form of N2. The accumulation of nitrogen in the biological and liquid phases was18%and4%, respectively. The nitrogen in the liquid phase is mainly present in the form of NO3-, and there is no N2O presence of in the exhaust gas. Only a small amount of nitrogen present in the form of NO2and CH4. About5%of the nitrogen is in the form of other types or experimental error.
The reaction rate of NO absorption capacity by ferrous EDTA (Fe(II)EDTA) solution and reduction by microorganism were studied in an scrubber-bioreactor system.The results show that the order of the four reaction rates in reactor is as follow: Fe(II)EDTA-NO reduction rate> Fe(II)EDTA oxidation rate>Fe(III)EDTA reduction rate> NO absorption rate,so the NO absorption process and Fe(III)EDTA reduction are key steps for NO removal efficiency in this integrated system.
The microbial community structure in the biological packed tower was analyses with the PCR-DGGE technology. The microbial species at the top of the tower was least due to water erosion, while the bottom layer had the largest micro-organisms and less species. The similarity of microbial community structure increased with the increase height of packed bed. The preliminary analysis results indicated that the microorganisms in the biofilm belonged to β-Proteobacterium and Pseudomonas. The denitrifier was dominanted in the biofilm.
Investigate the influence on the NO removal efficiency of some elements such as the concentration of O2, NO, SO2, flow rate of inlet gas and absorbents. that the result of the influence on NO removal efficiency of the concentration of O2, NO, SO2, flow rate of inlet gas and absorbents was obtained. The results showed that the Fe(II)EDTA /Fe(Ⅱ)Cit mixed system has the best technical parameters and economic benefits.
引文
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