典型危险废物在两段式回转窑焚烧系统内的热处置和结渣特性研究及其应用
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摘要
我国2009年的危险废物产生量达到1430万吨,由于危险废物形态复杂,回转窑焚烧是一种比较适宜的安全处置方式。目前对危险废物焚烧特性、灰渣特性的研究尚不深入,回转窑焚烧系统在运行过程中缺乏必要的指导,在实际应用中出现了危险废物焚烧效果不佳、回转窑内结渣、耐火材料腐蚀、污染物排放不达标等问题。依托国家高技术研究发展计划(863计划)重点项目课题“危险废物焚烧系统关键技术与示范”(2007AA061302)和浙江省重大科技专项“工业危险废物新型回转窑集成系统处置技术示范工程”(2007C13084),本文对几种典型危险废物的热解、燃烧特性开展了基础研究工作,并对危险废物焚烧处置工程应用进行试验研究,为现有的危险废物热处置研究提供有益的补充,为回转窑危险废物焚烧系统的运行优化提供支持。
本文首先运用化学热力学平衡模拟和试验研究对危险废物在不同热处置条件下的气体生成特性进行了研究。研究发现,危险废物热解产物主要是H20、C2H4、C2H2、H2和CO,随着温度的升高,热解气态产物出现进一步分解。在较低的过量空气系数条件下,危险废物的气化产物主要是CO、H2O、H2、和CH4,研究发现,少量O2有利于危险废物在热分解过程中CH4、H2和CO的生成。在危险废物热处置过程中,绝大部分C1元素在300-600℃之间以HCl的形式释放析出,危险废物焚烧过程中,S02是最主要的含S污染物。
利用热重-红外分析方法进行实验研究和动力学分析表明,危险废物燃烧过程的挥发份析出阶段与其热解过程的挥发份析出阶段具有相似的热分解特性,而氧气对危险废物的热分解具有明显的促进作用,使热分解温度提前,表观活化能降低。研究发现,危险废物热解气态产物的析出主要集中在200-500℃之间,大部分危险废物在700℃之前燃烬。高挥发份危险废物的热解气态产物析出较为集中,析出气体具有较高的浓度；高氮含量有机危险废物热解气中含有大量的HNCO,高硫危险废物热处置过程中的主要气态污染物是S02。有机化工污泥的固定碳燃烧阶段持续时间相对较长,且大部分失重都在固定碳燃烧阶段完成。实验研究发现,升温速率的提高对危险废物热解产物成分的影响较小
针对较高重金属含量的制革污泥的研究发现,其具有较好的燃烧特性。制革污泥在挥发份燃烧初期有少量有机酸析出,800℃时基本燃烬,超过900℃以后,制革污泥燃烧灰渣开始出现粘结现象。为避免制革污泥焚烧过程中出现结渣,并有效减少重金属的挥发,可以选择800℃为制革污泥的最佳燃烧温度。
本文利用计算流体软件,对危险废物在两段式回转窑焚烧系统内的燃烧过程进行了不同运行工况条件下的模拟。研究发现,在回转窑的后部区域,烟气流速存在明显的分层现象。在额定负荷和配风条件下,危险废物在回转窑内能够实现较为充分的燃烧,增加窑头部位的送风量以后,窑内烟气流速分层现象提前,窑内高温区域前移,危险废物在回转窑内的燃烧完全程度提高,二燃室的燃烧现象明显减弱。模拟研究表明,投用窑头助燃燃烧器可以在回转窑内部形成一个稳定的沿着回转窑轴向分布的高温区域,有助于促进窑内温度的稳定和危险废物在窑内的燃烧。
对危险废物焚烧处置工程应用的研究发现,两段式回转窑焚烧系统完全可以满足危险废物焚烧和污染物排放控制要求,稳定运行期间二噁英排放浓度只有0.016-0.035 TEQ ng/m3,但回转窑内存在较大程度的结渣隐患。危险废物焚烧飞灰呈现明显的小颗粒团聚特征,底渣质地致密,具有明显的烧结迹象,灰渣中部分重金属含量较高。通过对不同部位灰渣采样的分析,研究了危险废物在高温焚烧条件下的灰渣特性,以及烟气流动方向飞灰的形成过程和小颗粒的团聚过程,以及小颗粒在大颗粒表面富集的过程,为危险废物焚烧应用及污染物排放控制提供借鉴。
The hazardous waste output in China was 14.3 Mt in 2009. Incineration in rotary kiln is reasonable for hazardous waste treatment because of the complicated composition of hazardous wastes, while the farther investigation on combustion and slagging characteristics is necessary for application of the hazardous waste incineration. There are many problems in application of rotary kiln combustion such as incomplete combustion, ringing in kiln, corrosion to the refractory materials, and discharge of pollutants emission. Funded by National High Technology Research and Development Key Program of China (2007AA061302), Important Project on Science and Technology of Zhejiang Province of China (2007C13084), the basic characteristic of pyrolysis and combustion of typical hazardous waste were investigated and experimental studies were conducted in this paper, which is useful to hazardous waste thermal disposal and the operation optimization for incineration system.
The gaseous products of hazardous waste in pyrolysis and combustion at different condition were investigated by using thermodynamic equilibrium calculation and experimental study. The products were further decomposed with temperature increasing, and the main gaseous products in pyrolysis were H2O, C2H4, C2H2, H2 and CO. The main gaseous products in gasification at low air coefficient were CO, H2O, H2 and CH4. The generation of CH4, H2, CO were promoted by present of little O2. Most chlorine element in hazardous waste was emitted as HC1 in the temperature range of 300-600℃. SO2 is the most important sulfur containing gases product, while little SO2 were emitted during hazardous waste thermal disposal when air coefficient is lower than 0.6.
The similarity of thermal decomposition characteristics for the pyrolysis and low temperature stage during combustion was confirmed by TG-FTIR, and the decomposition was accelerated and advanced by present of O2. Most of the gaseous products in pyrolysis emitted during 200-500℃, and combustion of the hazardous waste almost finished before 700℃because of the low concentration of fixed carbon. The high-concentration gaseous products were emitted in a narrow temperature range during high volatile hazardous waste pyrolysis. Large amount of HNCO was emitted during high nitrogen hazardous waste pyrolysis, while SO2 is the most important gaseous product for high sulfur hazardous waste thermal disposal. The fixed carbon of organic chemical industry sludge burnt in a wide temperature range, and most of the weight lost in this stage. Heating rate has little influence on the gaseous products during hazardous waste pyrolysis.
The heavy metal sludge form tannery industry has good combustion characteristics compared with paper mill sludge and lake sludge. There was some organic acid gaseous product emitted at low temperature stage in tannery sludge combustion, and the combustion almost finished before 800℃. The combustion residue of tannery sludge was sintered above 900℃. For tannery sludge,800℃is a reasonable incineration temperature to control heavy metal volatilization.
The operation at different conditions of the hazardous waste two-stage incineration system consist of rotary kiln and secondary combustion chamber was simulated with Computational Fluid Dynamics code (FLUENT). The lamination of the velocity was obvious at the kiln end. Lamination of the velocity and the high-temperature zone in rotary kiln was advanced when the supplied air from the front-end increased. The proportion of the waste combustion in rotary kiln was enhanced when the air from the front-end increased. Stabilization of the combustion in kiln was strengthened by burner at the front-end.
Based on the on-site investigation on the application of hazardous waste incineration system consists of rotary kiln and secondary combustion chamber, it is confirmed that the two-stage incineration system is appropriate for complete combustion and gaseous pollutants control. The dioxins content in flow gas emission is 0.016-0.035 TEQ ng/m3 during the steady operation of the incineration system, while there was a tendency of combustion residue sintering in rotary kiln operation. The fly ash, which is agglomerated particle, exhibited the loose and cracked structure, while there is no large pore structure in bottom residue. Bottom residue from the hazardous waste incineration is rigidity, and the residue was melted in high temperature zone before it is flush off from the kiln. The particle agglomeration of the fly ash was confirmed by using the microstructure analysis on the ashes sampled from different position in the incineration and flue gas purification system. The research is useful for application of hazardous waste incineration and emission control.
本文首先运用化学热力学平衡模拟和试验研究对危险废物在不同热处置条件下的气体生成特性进行了研究。研究发现,危险废物热解产物主要是H20、C2H4、C2H2、H2和CO,随着温度的升高,热解气态产物出现进一步分解。在较低的过量空气系数条件下,危险废物的气化产物主要是CO、H2O、H2、和CH4,研究发现,少量O2有利于危险废物在热分解过程中CH4、H2和CO的生成。在危险废物热处置过程中,绝大部分C1元素在300-600℃之间以HCl的形式释放析出,危险废物焚烧过程中,S02是最主要的含S污染物。
利用热重-红外分析方法进行实验研究和动力学分析表明,危险废物燃烧过程的挥发份析出阶段与其热解过程的挥发份析出阶段具有相似的热分解特性,而氧气对危险废物的热分解具有明显的促进作用,使热分解温度提前,表观活化能降低。研究发现,危险废物热解气态产物的析出主要集中在200-500℃之间,大部分危险废物在700℃之前燃烬。高挥发份危险废物的热解气态产物析出较为集中,析出气体具有较高的浓度；高氮含量有机危险废物热解气中含有大量的HNCO,高硫危险废物热处置过程中的主要气态污染物是S02。有机化工污泥的固定碳燃烧阶段持续时间相对较长,且大部分失重都在固定碳燃烧阶段完成。实验研究发现,升温速率的提高对危险废物热解产物成分的影响较小
针对较高重金属含量的制革污泥的研究发现,其具有较好的燃烧特性。制革污泥在挥发份燃烧初期有少量有机酸析出,800℃时基本燃烬,超过900℃以后,制革污泥燃烧灰渣开始出现粘结现象。为避免制革污泥焚烧过程中出现结渣,并有效减少重金属的挥发,可以选择800℃为制革污泥的最佳燃烧温度。
本文利用计算流体软件,对危险废物在两段式回转窑焚烧系统内的燃烧过程进行了不同运行工况条件下的模拟。研究发现,在回转窑的后部区域,烟气流速存在明显的分层现象。在额定负荷和配风条件下,危险废物在回转窑内能够实现较为充分的燃烧,增加窑头部位的送风量以后,窑内烟气流速分层现象提前,窑内高温区域前移,危险废物在回转窑内的燃烧完全程度提高,二燃室的燃烧现象明显减弱。模拟研究表明,投用窑头助燃燃烧器可以在回转窑内部形成一个稳定的沿着回转窑轴向分布的高温区域,有助于促进窑内温度的稳定和危险废物在窑内的燃烧。
对危险废物焚烧处置工程应用的研究发现,两段式回转窑焚烧系统完全可以满足危险废物焚烧和污染物排放控制要求,稳定运行期间二噁英排放浓度只有0.016-0.035 TEQ ng/m3,但回转窑内存在较大程度的结渣隐患。危险废物焚烧飞灰呈现明显的小颗粒团聚特征,底渣质地致密,具有明显的烧结迹象,灰渣中部分重金属含量较高。通过对不同部位灰渣采样的分析,研究了危险废物在高温焚烧条件下的灰渣特性,以及烟气流动方向飞灰的形成过程和小颗粒的团聚过程,以及小颗粒在大颗粒表面富集的过程,为危险废物焚烧应用及污染物排放控制提供借鉴。
The hazardous waste output in China was 14.3 Mt in 2009. Incineration in rotary kiln is reasonable for hazardous waste treatment because of the complicated composition of hazardous wastes, while the farther investigation on combustion and slagging characteristics is necessary for application of the hazardous waste incineration. There are many problems in application of rotary kiln combustion such as incomplete combustion, ringing in kiln, corrosion to the refractory materials, and discharge of pollutants emission. Funded by National High Technology Research and Development Key Program of China (2007AA061302), Important Project on Science and Technology of Zhejiang Province of China (2007C13084), the basic characteristic of pyrolysis and combustion of typical hazardous waste were investigated and experimental studies were conducted in this paper, which is useful to hazardous waste thermal disposal and the operation optimization for incineration system.
The gaseous products of hazardous waste in pyrolysis and combustion at different condition were investigated by using thermodynamic equilibrium calculation and experimental study. The products were further decomposed with temperature increasing, and the main gaseous products in pyrolysis were H2O, C2H4, C2H2, H2 and CO. The main gaseous products in gasification at low air coefficient were CO, H2O, H2 and CH4. The generation of CH4, H2, CO were promoted by present of little O2. Most chlorine element in hazardous waste was emitted as HC1 in the temperature range of 300-600℃. SO2 is the most important sulfur containing gases product, while little SO2 were emitted during hazardous waste thermal disposal when air coefficient is lower than 0.6.
The similarity of thermal decomposition characteristics for the pyrolysis and low temperature stage during combustion was confirmed by TG-FTIR, and the decomposition was accelerated and advanced by present of O2. Most of the gaseous products in pyrolysis emitted during 200-500℃, and combustion of the hazardous waste almost finished before 700℃because of the low concentration of fixed carbon. The high-concentration gaseous products were emitted in a narrow temperature range during high volatile hazardous waste pyrolysis. Large amount of HNCO was emitted during high nitrogen hazardous waste pyrolysis, while SO2 is the most important gaseous product for high sulfur hazardous waste thermal disposal. The fixed carbon of organic chemical industry sludge burnt in a wide temperature range, and most of the weight lost in this stage. Heating rate has little influence on the gaseous products during hazardous waste pyrolysis.
The heavy metal sludge form tannery industry has good combustion characteristics compared with paper mill sludge and lake sludge. There was some organic acid gaseous product emitted at low temperature stage in tannery sludge combustion, and the combustion almost finished before 800℃. The combustion residue of tannery sludge was sintered above 900℃. For tannery sludge,800℃is a reasonable incineration temperature to control heavy metal volatilization.
The operation at different conditions of the hazardous waste two-stage incineration system consist of rotary kiln and secondary combustion chamber was simulated with Computational Fluid Dynamics code (FLUENT). The lamination of the velocity was obvious at the kiln end. Lamination of the velocity and the high-temperature zone in rotary kiln was advanced when the supplied air from the front-end increased. The proportion of the waste combustion in rotary kiln was enhanced when the air from the front-end increased. Stabilization of the combustion in kiln was strengthened by burner at the front-end.
Based on the on-site investigation on the application of hazardous waste incineration system consists of rotary kiln and secondary combustion chamber, it is confirmed that the two-stage incineration system is appropriate for complete combustion and gaseous pollutants control. The dioxins content in flow gas emission is 0.016-0.035 TEQ ng/m3 during the steady operation of the incineration system, while there was a tendency of combustion residue sintering in rotary kiln operation. The fly ash, which is agglomerated particle, exhibited the loose and cracked structure, while there is no large pore structure in bottom residue. Bottom residue from the hazardous waste incineration is rigidity, and the residue was melted in high temperature zone before it is flush off from the kiln. The particle agglomeration of the fly ash was confirmed by using the microstructure analysis on the ashes sampled from different position in the incineration and flue gas purification system. The research is useful for application of hazardous waste incineration and emission control.
引文
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