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1.
In order to investigate the CH4 and CO2 fluxes across the water-gas interface and identify their controlling factors, four diel field campaigns and one monthly sampling campaign during June 2010-May 2011 were carried out at a site near the Three Gorges Dam, China. The averaged CH4 and CO2 fluxes across the air-water interface from the site were much less than those reported from reservoirs in tropic and temperate regions, and from the natural river channels of the Yangtze River. CH4 Fluxes at the site were very low compared to most other reservoirs or natural lakes. One of the most important reasons may be due to the oxidation of CH4 in the water column owing to the great water depth and high DO in water in the Three Gorges Reservoir. The averaged monthly CH4 and CO2 fluxes at the site during the observation year were 0.05 mg/(m^2·hr) and 104.43 mg/(m^2·hr) respectively with the maximum occurred in July 2010. The monthly CO2 fluxes during the observation year were positively correlated to the surface water temperature, and negatively correlated to the air pressure and the surface water pH. The CO2 flux showed a positive correlation with DOC to some extent, although not significantly, which indicated that allochthonous organic C was a major source of CO2 and biogeochemical processes in this reservoir were C-limited. The significantly positive correlation between the reservoir outflow and the seasonal gas flux indicate the disturbance condition of the water body dominated the seasonal gas emission.  相似文献   

2.
氨水混合吸收剂脱除CO2实验研究   总被引:2,自引:1,他引:1  
氨水作为一种很有应用前景的CO2化学吸收剂,存在吸收速率慢的问题.使用湿壁塔实验台,考察了不同种类的添加剂(MEA、PZ、1-MPZ、2-MPZ)对氨水吸收CO2速率的影响.结果表明,4种添加剂均能明显提高氨水吸收CO2的速率,其中PZ具有最好的促进效果.0、0.1、0.3和0.5 mol·mol-1负荷下,3 mol·L-1NH3+0.3 mol·L-1PZ溶液的总传质系数(KG)分别是3 mol·L-1NH3溶液在相应负荷下的3、3.2、3.2和2.9倍.改变反应温度、添加剂量、PZ浓度等条件对基于NH3/PZ混合吸收剂吸收CO2的反应过程进行实验,得到了其在不同条件下的KG,初步探讨CO2吸收的反应机制,并计算出准一级反应速率常数为42.7 m3·(mol·s)-1.  相似文献   

3.
CO2 is the main greenhouse gas which causes global climatic changes on larger scale. Many techniques have been utilised to capture CO2. Membrane gas separation is a fast growing CO2 capture technique, particularly gas separation by composite membranes. The separation of CO2 by a membrane is not just a process to physically sieve out of CO2 through the controlled membrane pore size. It mainly depends upon diffusion and solubility of gases, particularly for composite dense membranes. The blended components in composite membranes have a high capability to adsorb CO2. The adsorption kinetics of the gases may directly affect diffusion and solubility. In this study, we have investigated the adsorption behaviour of CO2 in pure and composite membranes to explore the complete understanding of diffusion and solubility of CO2 through membranes. Pure cellulose acetate (CA) and cellulose acetate-titania nanoparticle (CA-TiO2) composite membranes were fabricated and characterised using SEM and FTIR analysis. The results indicated that the blended CA-TiO2 membrane adsorbed more quantity of CO2 gas as compared to pure CA membrane. The high CO2 adsorption capacity may enhance the diffusion and solubility of CO2 in the CA-TiO2 composite membrane, which results in a better CO2 separation. The experimental data was modelled by Pseudo first-order, pseudo second order and intra particle diffusion models. According to correlation factor R2, the Pseudo second order model was fitted well with experimental data. The intra particle diffusion model revealed that adsorption in dense membranes was not solely consisting of intra particle diffusion.  相似文献   

4.
Aqueous ammonia (NH3) solution can be used as an alternative absorption for the control of CO2 emitted from flue gases due to its high absorption capacity, fast absorption rate and low corrosion problem. The emission of CO2 from iron and steel plants requires much attention, as they are higher than those emitted from power plants at a single point source. In the present work, low concentration ammonia liquor, 9 wt.%, was used with various additives to obtain the kinetic properties using the blast furnace gas model. Although a solution with a high ammonia concentration enables high CO2 absorption efficiency, ammonium ions are lost as ammonia vapor, resulting in reduced CO2 absorption due to the lower concentration of the ammonia absorbent. To decrease the vaporization of ammonia, ethylene glycol, glycerol and glycine, which contain more than one hydroxyl radical, were chosen. The experiments were conducted at 313 K similar to the CO2 absorption conditions for the blast furnace gas model.  相似文献   

5.
Aqueous 1,8-diamino-p-menthane (KIER-C3) and commercially available amine solutions were tested for CO2 absorption. A 2-amino- 2-methyl-1-propanol (AMP) solution with an addition of KIER-C3 showed 9.3% and 31.6% higher absorption rate for CO2 than the AMP solution with an addition of monoethanolamine (MEA) and ammonia (NH3), respectively. The reaction rate constant for CO2 absorption by the AMP/KIER-C3 solution was determined by the following equation: k2,AMP/C3 = 7.702×106 exp (-2248.03/T). A CO2 loading ratio of the AMP/KIER-C3 solution was also 2 and 3.4-times higher than that of the AMP/NH3 solution and the AMP/MEA solution, respectively. Based on the experimental results, KIER-C3 may be used as an excellent additive to increase CO2 absorption capability of AMP.  相似文献   

6.
The effects of gas compositions and reaction conditions on NO conversion by positive streamer discharge were experimentally investigated by using a link tooth wheel-cylinder reactor. The results showed that NO conversion increased with increasing O2 concentration and NH3 concentration, but decreased with increasing inlet NO concentration and gas flow rate. The addition of CO2 or H2O to the feed gas promoted NO conversion by increasing the maximum discharge voltage, and NH4NO3 was formed in the presence of NH3. There was a most suitable range interval between discharge tooth wheels if both NO conversion and energy consumption were considered. Increasing applied voltage resulted in the increase in the amount of O3 generated by streamer discharge.  相似文献   

7.
通过水热法合成盘状ZnO,并在其表面负载Cu得到Cu/盘状ZnO模型催化剂,将不同气氛下(5%CO/Ar、2.5%H_2/2.5%CO/Ar、5%H_2/Ar,分别记为CZ-5CO、CZ-2.5H_2-2.5CO、CZ-5H_2)还原的模型催化剂用于逆水煤气变换反应.对催化剂进行热重分析(TGA)、X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、原位紫外拉曼光谱(in situ UV-Raman)表征.结果表明,不同的还原气氛可得到不同尺寸的Cu颗粒及不同缺陷浓度的Cu-ZnO界面.CO_2程序升温脱附(CO_2-TPD)结果表明,不同的Cu-ZnO界面具有不同的CO_2活化能力.其中CZ-5H_2形成的Cu-ZnO界面对CO_2活化能力最强,表现出最佳的逆水煤气变换反应活性;CZ-5CO具有更多的表面缺陷可能是由于存在Cu_3Zn合金,但Cu-ZnO界面上CO_2的吸附容量降低,导致逆水煤气变换反应活性低;CZ-2.5H_2-2.5CO的活性介于CZ-5H_2与CZ-5CO之间,界面对CO_2的活化量也介于两者之间.  相似文献   

8.
Minimizing soil ammonia (NH3) and nitrous oxide (N2O) emission factors (EFs) has significant implications in regional air quality and greenhouse gas (GHG) emissions besides nitrogen (N) nutrient loss. The aim of this study was to investigate the impacts of different N fertilizer treatments of conventional urea, polymer-coated urea, ammonia sulfate, urease inhibitor (NBPT, N-(n-butyl) thiophosphoric triamide)-treated urea, and nitrification inhibitor (DCD, dicyandiamide)-treated urea on emissions of NH3 and GHGs from subtropical wheat cultivation. A field study was established in a Cancienne silt loam soil. During growth season, NH3 emission following N fertilization was characterized using active chamber method whereas GHG emissions of N2O, carbon dioxide (CO2), and methane (CH4) were by passive chamber method. The results showed that coated urea exhibited the largest reduction (49%) in the EF of NH3-N followed by NBPT-treated urea (39%) and DCD-treated urea (24%) over conventional urea, whereas DCD-treated urea had the greatest suppression on N2O-N (87%) followed by coated urea (76%) and NBPT-treated urea (69%). Split fertilization of ammonium sulfate-urea significantly lowered both NH3-N and N2O-N EF values but split urea treatment had no impact over one-time application of urea. Both NBPT and DCD-treated urea treatments lowered CO2-C flux but had no effect on CH4-C flux. Overall, application of coated urea or urea with NPBT or DCD could be used as a mitigation strategy for reducing NH3 and N2O emissions in subtropical wheat production in Southern USA.  相似文献   

9.
Nitrous oxide emissions from black soils with different pH   总被引:1,自引:0,他引:1  
N2O fluxes as a function of incubation time from soil with different available N contents and pH were determined. Cumulative carbon dioxide (CO2) emissions were measured to indicate soil respiration. A 144-hr incubation experiment was conducted in a slightly acidic agricultural soil (pHH2O 5.33) after the pH was adjusted to four different values (3.65, 5.00, 6.90 and 8.55). The experiments consisted of a control without added N, and with NH4+-N and NO3--N fertilization. The results showed that soil pH contributed significantly to N2O flux from the soils. There were higher N2O emissions in the period 0-12 hr in the four pH treatments, especially those enhanced with N-fertilization. The cumulative N2O-N emission reached a maximum at pH 8.55 and was stimulated by NO3--N fertilization (70.4 μg/kg). The minimum emissions appeared at pH 3.65 and were not stimulated by NO3--N or NH4+-N fertilization. Soil respiration increased significantly due to N-fertilization. Soil respiration increased positively with soil pH (R2 = 0.98, P < 0.01). The lowest CO2-C emission (30.2 mg/kg) was presented in pH 3.65 soils without N-fertilization. The highest CO2-C emissions appeared in the pH 8.55 soils for NH4+-N fertilization (199 mg/kg). These findings suggested that N2O emissions and soil respiration were significantly influenced by low pH, which strongly inhibits soil microbial nitrification and denitrification activities. The content of NO3--N in soil significantly and positively affected the N2O emissions through denitrification.  相似文献   

10.
蒋滔  郭劲松  李哲  方芳  白镭  刘静 《环境科学》2012,33(5):1463-1470
水电是具有显著减排效益的清洁能源形式,但水库潜在的温室气体效应近年来备受关切,在一定程度上影响了人们对水库清洁能源属性的认识.本研究分别于2010年8月水库低水位运行期及12月高水位运行期,对三峡库区典型支流——澎溪河上游温泉至下游双江6个沿程断面进行水样的采集及温室气体通量的监测研究.结果表明,在河流纵向上,表层水体水温、pH逐渐沿程增加,而CO2分压(pCO2)和碱度(TA)则有相反趋势.在低水位的8月,开县以下断面CO2通量为负,且浮游植物可能是控制水体CO2通量及营养盐的关键因素之一.澎溪河回水区CO2通量相对天然河道背景断面(温泉)平均降低了3.26 mmol.(m2.h)-1,而CH4通量却大幅度增加了.在高水位运行的12月,澎溪河各断面均为CO2释放通量,CH4通量相比低水位则明显降低.相比较天然河道的温泉断面,澎溪河回水区在高水位运行状态下CO2与CH4通量分别增加了4.16mmol.(m2.h)-1和0.007 mmol.(m2.h)-1.初步的净通量分析发现,该水域较加拿大实验水库的净通量特征低.  相似文献   

11.
In this work we present the experimental results of absorption rates and absorption capacity for the CO2 absorption by ammonia (NH3) aqueous solutions. Experiments are carried out in a thermoregulated Lewis-type cell reactor and are achieved in temperature and concentration ranges of 278–303 K and 2–5wt.% NH3 respectively. The obtained values for absorption kinetic rates and absorption capacity are compared with those available for alkanolamine solvents, commonly used to absorb CO2. In order to achieve this comparison, data available in studies about alkanolamine solvents at 303–333 K and 5–50wt.% for alkanolamines solutions were considered. Results show that CO2 absorption by NH3 is faster than the one carried out by MDEA, except for 2wt.% NH3 at 288 K. At 278 K and using aqueous solutions of 3wt.% NH3, the absorption rate is almost identical to the one reached with MDEA solvent. The highest absorption capacity, also compared with alkanolamine solution, is reached with aqueous solutions of 5wt.% NH3 at 278 K and 303 K.  相似文献   

12.
畜禽粪肥在贮存阶段养分损失严重,是CO_2、CH_4、NH_3和N_2O等大气污染物的重要排放来源.本文采用室内培养方法,研究了添加黄土、秸秆、生物炭和膨润土对猪粪贮存过程中氨气及温室气体排放的影响.结果表明,添加10%用量的生物炭和膨润土处理的CO_2累积排放量与不添加任何添加物的猪粪对照相比分别降低了15.4%和20.9%,N_2O累积排放量分别降低了19.8%和37.6%.添加膨润土处理的NH_3损失量显著增加,但添加生物炭和膨润土处理的综合温室效应与猪粪对照相比均显著降低.添加10%秸秆处理的CH_4和NH_3累积排放量分别较猪粪对照降低了56.8%和95.8%,但其综合温室效应与对照相比差异不显著.模拟黄土垫圈过程添加黄土处理的氨气及温室气体累积排放量均显著降低,综合温室效应显著低于其他处理(p0.05).可见,黄土垫圈是保蓄粪肥碳、氮养分的有效措施,猪粪贮存阶段添加少量生物炭、膨润土对于减少粪肥综合温室效应具有积极作用.  相似文献   

13.
为确定规模化笼养肉鸡生产过程NH3、N2O、CH4和CO2的排放因子,并探讨不同生长阶段排放特征,本研究选择山东某商业化肉鸡养殖场,利用INNOVA 1312多气体分析仪-连续采样测试系统和风机风量现场测定系统(FANS),对肉鸡舍NH3、N2O、CH4和CO2的排放进行为期42 d的测定,确定了肉鸡整个生产过程气体的平均排放因子和累积排放因子.结果表明,整个肉鸡生产过程中NH3排放因子呈现出先升高后降低的趋势,变化范围在8.5~342.1 mg·(d·bird)-1,平均为137.9mg·(d·bird)-1[48.6 g·(d.AU)-1],CH4和CO2排放因子随着日龄的增加而增大,CH4排放因子的变化范围在19.5~351.9mg·(d·bird)-1之间,平均为154.5 mg·(d·bird)-1[54.4 g·(d.AU)-1],CO2的排放因子在2.2~152.9 g·(d·bird)-1之间变化,平均为65.9 g·(d·bird)-1[23.2 kg·(d.AU)-1],整个生产过程没有监测到N2O的排放;肉鸡的NH3累计排放因子为(5.65±1.02)g·(bird·life cycle)-1,第1阶段(0~17 d)、第2阶段(18~27 d)和第3生长阶段(28~42 d)氨气排放占总排放的比例分别为33.6%、36.4%和29.9%,第2阶段的NH3累计排放因子显著高于第1和第3生长阶段;CH4和CO2的累计排放因子分别为(6.30±0.16)g·(bird·life cycle)-1和(2.68±0.18)kg·(bird·life cycle)-1,第3阶段的CH4和CO2累计排放因子显著大于1和2阶段,占总排放量的50%以上.研究结果为控制气体排放提供了数据基础.  相似文献   

14.
为揭示好氧段气水比对缺氧/好氧生物滤池(Anoxic/Oxic Biofilter,A/O-BF)脱氮的影响机理,采用A/O-BF处理低碳氮比农村生活污水,结合实时荧光定量聚合酶链式反应技术,对比研究了好氧段气水比为4∶1、2∶1和1∶1时A/O-BF的脱氮效能和微生物群落变化特征.结果表明:当气水比为4∶1时,A/O...  相似文献   

15.
Slurries are a significant source of CH4, NH3 and N2O emissions to the atmosphere. The research project aimed at quantifying CH4, NH3 and N2O emissions from liquid manure stores and after manure application under field conditions. The influence of the manure treatment options “no treatment”, “slurry separation”, “anaerobic digestion”, “slurry aeration” and “straw cover” on the emission level was investigated. Approximately 10 m3 of differently treated slurry were stored in pilot scale slurry tanks. Emissions were followed for c. 80 days. After the storage period, slurries were applied to permanent grassland. Greenhouse gas emissions from slurry were mainly caused by methane emissions during storage and by nitrous oxide emissions after field application of manures. Mitigation of GHG emissions can be achieved by a reduction in slurry dry matter and easily degradable organic matter content. Ammonia emissions mainly occurred after field application. Untreated slurry emitted 226.8 g NH3 m−3 and 92.4 kg CO2 eq. m−3 (storage and field application). Slurry separation (liquid fraction and composting of the solid fraction) resulted in NH3 losses of 402.9 g m−3 and GHG losses of 58.5 kg CO2 eq. m−3. Anaerobic digestion was a very effective means to reduce GHG emissions. 37.9 kg CO2 eq. m−3 were lost. NH3 emissions were similar to those from untreated slurry. Covering the slurry store with a layer of chopped straw instead of a wooden cover increased NH3 emissions to 320.4 g m−3 and GHG emissions to 119.7 kg CO2 eq. m−3. Slurry aeration nearly doubled NH3 emissions compared to untreated slurry. GHG emissions were reduced to 53.3 kg CO2 eq. m−3.  相似文献   

16.
Selective catalytic reduction (SCR) denitration may increase the emission of NH4+ and NH3. The removal and transformation characteristics of ammonium sulfate aerosols and ammonia slip during the wet flue gas desulfurization (WFGD) process, as well as the effect of desulfurization parameters, were investigated in an experimental system equipped with a simulated SCR flue gas generation system and a limestone-based WFGD system. The results indicate that the ammonium sulfate aerosols and ammonia slip in the flue gas from SCR can be partly removed by slurry scrubbing, while the entrainment and evaporation of desulfurization slurry with accumulated NH4+ will generate new ammonium-containing particles and gaseous ammonia. The ammonium-containing particles formed by desulfurization are not only derived from the entrainment of slurry droplets, but also from the re-condensation of gaseous ammonia generated by slurry evaporation. Therefore, even if the concentration of NH4+ in the desulfurization slurry is quite low, a high level of NH4+ was still contained in the fine particles at the outlet of the scrubber. When the accumulated NH4+ in the desulfurization slurry was high enough, the WFGD system promoted the conversion of NH3 to NH4+ and increased the additional emission of primary NH4+ aerosols. With the decline of the liquid/gas ratio and flue gas temperature, the removal efficiency of ammonia sulfate aerosols increased, and the NH4+ emitted from entrainment and evaporation of the desulfurization slurry decreased. In addition, the volatile ammonia concentration after the WFGD system was reduced with the decrease of the NH4+ concentration and pH values of the slurry.  相似文献   

17.
汪军  王德建  张刚  王远 《环境科学》2013,34(1):27-33
利用原状土柱在田间试验条件下,比较了麦秸还田下乌栅土和黄泥土稻季氮素氨挥发损失规律,每种试验土壤均设对照、氮肥、氮肥加麦秆这3个处理,同步测定施肥后氨挥发、田面水铵态氮浓度与pH、以及表层土壤Eh.结果表明,乌栅土氨挥发速率及其累积氨挥发量显著高于黄泥土,两种土壤的稻季平均氨挥发的氮素损失量分别为41.8 kg·hm-2和11.2kg·hm-2,分别占氮肥用量的15.2%和3.8%;在3个施肥时期中,分蘖肥期氨挥发损失率最高,乌栅土和黄泥土分别占氮肥用量的29.4%和8.3%;麦秸还田显著增加了氮肥的氨挥发损失,麦秸还田下乌栅土和黄泥土稻季氨挥发损失比单施氮肥处理分别增加了19.8%和20.6%.两种土壤氨挥发速率均与田面水NH4+-N浓度、pH呈正相关关系,但与表层土壤Eh的关系还需进一步研究.  相似文献   

18.
罗佳宸  李思悦 《环境科学》2018,39(11):5217-5226
为研究河流水-气界面CO_2通量的季节和日变化特征;于2016年7月15~17日以及2017年11月4~6日对三峡库区嘉陵江支流竹溪河进行定点定时采集表层水样,并同步监测关键环境因子,采用亨利定律结合薄边界层模型计算其水-气界面CO_2通量F(CO_2).结果表明,竹溪河表层水CO_2分压p(CO_2)及界面CO_2脱气通量呈现出显著的日间和季节变化,以及明显的日内变化特征:在上午09:00前后达到释放高峰,随后波动下降;水-气界面CO_2通量日间均值分别为(100. 9±31. 6)、(78. 6±12. 1)、(83. 9±29. 7)、(137. 5±42. 1)、(147. 6±34. 0)、(132. 4±21. 7) mmol·(m~2·d)~(-1);并表现出夏季表层水体CO_2释放通量明显低于秋季,其均值分别为(87. 8±27. 5) mmol·(m~2·d)~(-1)和(139. 2±34. 0) mmol·(m~2·d)~(-1);总体表现出大气CO_2源的特征.竹溪河p(CO_2)和F(CO_2)受到诸多环境因子的影响,相关分析表明,pH、碱度、水温和气温是主要环境影响因子,CO_2释放通量可以用pH和碱度预测.  相似文献   

19.
Aerobic composting is a method for the sanitary disposal of human feces as is used in bio-toilet systems. As the products of composting can be utilized as a fertilizer, it would be beneficial if the composting conditions could be more precisely controlled for the retention of fecal nitrogen as long as possible in the compost. In this study, batch experiments were conducted using a closed aerobic thermophilic composting reactor with sawdust as the bulk matrix to simulate the condition of a bio-toilet for the sanitary disposal of human feces. Attention was paid to the characteristics of nitrogen transformation. Under the controlled conditions of temperature at 60°C, moisture content at 60%,anda continuous air supply, more than 70% fecal organic removal was obtained, while merely 17% fecal nitrogen loss was observed over a two-week composting period. The nitrogen loss was found to occur mainly in the first 24 h with the rapid depletion of inorganic nitrogen but with an almost unchanged organic nitrogen content. The fecal NH4-N which was the main component of the inorganic nitrogen ( > 90%) decreased rapidly in the first day, decreased at a slower rate over the following days, and finally disappeared entirely. The depletion of NH4-N was accompanied by the accumulation of NH3 gas in the ammonia absorber connected to the reactor. A mass balance between the exhausted NH3 gas and the fecal NH4-N content in the first 24 hours indicated that the conversion of ammonium into gaseous ammonia was the main reason for nitrogen loss. Thermophilic composting could be considered as a way to keep a high organic nitrogen content in the compost for better utilization as a fertilizer.  相似文献   

20.
利用生物炭吸附面源污染水体NH4+-N并将其进行还田可实现此氮资源由水体到农田的安全有效迁移,而探索负载NH4+-N生物炭对N2O-N排放和NH3-N挥发的影响则对于减施化肥和降低土壤氮素损失意义重大.本研究采用土柱试验,设置4个处理:对照(不施氮肥,CK)、单施化肥(NPK)、负载氮+化学磷钾肥(N-BC+PK)和生物炭+化肥(BC+NPK).结果表明,相较NPK和BC+NPK处理,N-BC+PK处理N2O-N累积排放量、NH3-N累积挥发量、气态氮素累积损失量(以N计)分别显著降低了33.62%和24.64%、70.64%和79.29%、64.97%和73.75%(P<0.05).特别需要说明的是,BC+NPK处理相比NPK处理显著增加了NH3-N累积挥发量(P<0.05).综上所述,负载NH4+-N生物炭可显著减少N2O-N排放和NH3-N挥发,且其减排效果显著优于传统的生物炭化肥配施.本研究结果将为富营养化水体NH4+-N农田回用和土壤气态氮素减排提供理论依据和数据支持.  相似文献   

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