用循环流化床焚烧排水污泥时氮氧化物的生成特性

人们已注意到N₂O既是温室气体之一,又是同温层中破坏臭氧的重要物质。N₂O在循环流化床（CFB）燃烧系统中会大量产生,由于近年来作为废物燃烧器的CFB被广泛地应用,因此废物燃烧过程中N₂O生成特性研究已经成为新的焦点。1995年12月,在一小型石英CFB燃烧系统中观察了活性污泥燃烧。试验结果显示:①在850℃时N₂O排放超过1830 mg/m3;②活性污泥中N向NO和N₂O的转换率与煤炭相比低,③N₂O的排放受烟气中O₂浓度的影响。      

冬季太湖草、藻型湖区N2O的生成与排放特征

对太湖典型草（包括沉水植物及挺水植物湖区）、藻型湖区水-气界面N₂O排放通量、水柱溶存浓度、泥-水界面通量以及3个湖区的水柱及沉积物理化性质进行了原位观测及实验室分析研究,并针对影响N₂O生成与排放的主要环境因子进行了室内的微环境模拟试验.研究结果表明：水-气界面N₂O释放通量及泥-水界面N₂O释放通量为藻型湖区 > 沉水植物湖区 > 挺水植物湖区（（123.10±11.43）μg/（m²·h）,（79.19±4.90）μg/（m²·h）,（53.45±4.22）μg/（m²·h）和（29.60±0.20）μmol/（m²·h）,（10.89±1.66）μmol/（m²·h）,（3.83±0.30）μmol/（m²·h））;水体溶存N₂O浓度均为藻型湖区 > 挺水植物湖区 > 沉水植物湖区（（0.0247±0.0003）μmol/L,（0.0236±0.0003）μmol/L,（0.0219±0.0001）μmol/L）;室内微环境实验结果表明：冬季升高温度能够显著地提高N₂O的生成潜力,高盐度对3种生态类型湖区沉积物N₂O的生成速率总体表现出抑制作用,藻型湖区及挺水植物湖区沉积物N₂O释放潜力在添加Cl^-组明显高于控制组,氮盐度过高会抑制沉积物N₂O产生,而沉水植物湖区沉积物N₂O产生受到抑制;随添加NH+4-N和NO-3-N等营养盐浓度升高,藻型湖区及沉水植物湖区沉积物中N₂O生成速率增加,挺水植物湖区N₂O生成速率降低,而乙酸盐作为微生物活动的碳源和能源对N₂O生成表现出抑制作用.冬季太湖典型草、藻型湖区N₂O排放存在显著差异,冬季草/藻型湖区N2O生成主要受冬季低温的限制,另外也受水柱无机氮形态及浓度的影响.     

水稻成熟衰老期叶际及根际氮氧化物排放的光控机制

为研究水稻成熟衰老期叶际及根际NOGs(nitrogen oxides gases, 氮氧化物)排放的光控机制,在同步测定条件下,采用密闭箱法,研究了不同光质(黄、绿、白、红、蓝光)、光强〔0.00、(50.00±2.35)(75.00±2.32)(100.00±3.89) μmol/(m2·s)〕对水稻成熟衰老期叶际及根际NOGs排放的影响. 结果表明:在相同氮源〔NH₄NO₃-N,ρ(N)为90 mg/L〕下,日间光强为(75.00±2.32) μmol/(m2·s)时,水稻成熟衰老期叶际N₂O和NO的平均排放速率分别为18.09、0.39 μg/(pot·h),二者排放量分别占各自总排放量的28.88%、30.78%;在(100.00±3.89)μmol/(m2·s)光强条件下,叶际N₂O和NO的平均排放速率则分别为23.27、0.50 μg/(pot·h),二者排放量分别占各自总排放量的36.74%、27.92%. 在0.00～(100.00±3.89)μmol/(m2·s)日间光强下,水稻叶际及根际N₂O和NO排放随随光强增加而增强,但不同光照条件下水稻叶际及根际均无明显的NO₂净排放作用. 在光强一致〔(20.00±0.48)μmol/(m2·s)〕条件下,同期黄、绿、白、红、蓝光处理的水稻叶际N₂O平均排放速率分别为24.90、15.46、13.85、16.40和19.77 μg/(pot·h),红、蓝光在抑制水稻叶际N₂O及根际NO排放的同时,也促进了水稻根际N₂O的排放. 研究显示,水稻成熟衰老期叶际及根际NOGs排放均以N₂O为主,叶际N₂O的排放可以反映根际N₂O的排放情况. 光照越强,NOGs排放就越明显. 适度控制日间光强并增加红、蓝光比例,可抑制N₂O和NO排放.      

内蒙古河套灌区盐碱土壤N2O排放特征

选择内蒙古河套灌区强度盐碱土壤S₁[电导率（EC）2.60dS/m]和轻度盐碱土壤S₂[电导率（EC） 0.74dS/m]为研究对象,2014~2016年,利用静态箱法3年野外原位观测试验,研究盐碱土壤氧化亚氮（N₂O）排放通量.结果表明：2种不同盐碱程度土壤N₂O排放每年均存在显著差异,轻度盐碱土壤N₂O累积排放量低;随EC升高,土壤盐碱程度加重,土壤N₂O累积排放量升高.2014~2016年作物生长季（4~11月）轻度盐碱土壤N₂O累积排放量分别为180.6,167.6,118.2mg/m²;强度盐碱土壤N₂O累积排放量比轻度盐碱土壤分别增加19%、26%和45%,修复盐碱土壤成为减缓盐碱土壤N₂O累积排放的重要农艺措施.     

废水生物脱氮过程中N2O排放数学模型研究进展

氧化亚氮(N₂O)的温室效应比CO₂强265倍,可从废水生物脱氮过程中产生并直接排放,如果不对其加以控制,会显著增加污水处理厂的碳足迹。N₂O排放的数学建模对于深入解析N₂O产生机制、量化N₂O排放、优化生物脱氮工艺和制定N₂O减排策略具有重要意义。结合当前国内外研究现状,阐述了废水生物脱氮过程中N₂O产生机制;归纳了基于不同机制建立的N₂O数学模型,包括氨氧化细菌(ammonia-oxidizing bacteria,AOB)经过羟胺氧化途径和AOB反硝化途径产生N₂O模型、异养反硝化途径产生N₂O模型以及耦合AOB和异养反硝化细菌产生N₂O模型;总结了新型生物脱氮系统N₂O模型,实际工程应用情况及校准N₂O数学模型中存在的问题;并对今后N₂O数学模型的研究方向进行了展望。     

温度和氨氮浓度对水体N2O释放的影响

氧化亚氮的释放已经成为了一个全球性的环境问题,水体中N₂O的释放量会随着氮含量的增加而增加.本文通过微宇宙系统的构建,分析氮的转化过程和氮转化基因的变化,并结合结构方程模型分析了温度、氨氮含量对水体N₂O释放的贡献.研究结果发现氨氧化古菌和反硝化细菌丰度均与N₂O释放呈正相关,表明水体中的硝化和反硝化作用都会造成N₂O的释放.氨氮浓度的升高并不直接促进N₂O的释放,而温度和通过硝化作用产生的硝态氮对N₂O的释放有促进作用.此外,硝化速率通过促进亚硝态氮和反硝化菌的丰度而间接地促进N₂O的释放.     

深圳再生水补水河流溶解N2O空间分布和产生机制

为了探究在再生水回补城市河流的条件下河流N₂O的微生物产生过程及其空间变化特征,以深圳市西乡河为研究对象,分析了河水中c（溶解性N₂O）、c（NH₄+-N）、c（NO₃--N）、δ15Nbulk-N₂O、δ18O-N₂O、同位素异位体位嗜值（site preference,SP）及其他环境因子,并基于端元混合模型和同位素分馏模型定量计算硝化和反硝化作用对河水中N₂O贡献百分比.结果表明:①随着流速降低,西乡河河水从上游的好氧环境逐渐发育成中下游的厌氧环境.②再生水进入西乡河后河水c（溶解性N₂O）从1.36 μmol/L沿程降至0.19 μmol/L;相关性分析表明,影响c（溶解性N₂O）的主要因素为ρ（DO）（R2=0.800,P < 0.01）和c（CH₄）（R2=-0.736,P < 0.01）.③硝化和反硝化作用对河水中N₂O贡献率分别为14.36%~80.53%和19.47%~85.64%;N₂O的来源在好氧河段中以硝化作用为主,在厌氧河段则以反硝化作用为主;N₂O还原成N₂的比例与ρ（DO）具有显著负相关关系（R2=-0.782,P < 0.01）.研究显示,再生水回补城市河流引入了较高质量浓度的N₂O和NO₃--N,而河道的厌氧环境促进河水中N₂O还原成N₂,下游河流成为N₂O的汇.      

引江济太对太湖贡湖湾氧化亚氮通量的影响

选取引江济太工程中长江来水进入太湖第一站的贡湖湾为研究对象,基于2011年11月~2013年8月在贡湖湾的逐月野外调查,同时以湖心水域为参考,探讨引江济太对湖体N₂O通量的影响.结果表明,贡湖湾N₂O排放通量要显著高于湖心排放量,其N₂O通量均值分别为6.9,2.1μmol/（m²·d）,但在非引水期间2个湖区的N₂O通量无显著差异.贡湖湾和湖心N₂O通量呈现明显的季节变化,且均与水温呈显著负相关关系,但因受外源来水的影响,贡湖湾N₂O通量的温度依赖程度相对较低.另外,2个湖区的N₂O通量还与营养盐等因素有关.总体上,外源引水提高了贡湖湾N₂O排放通量,但考虑到湖泊N₂O通量受到内部和外部因子的综合协同影响,外源引水对湖泊N₂O通量的具体调控机理还需要进一步探讨.     

河湖氧化亚氮(N2O)温室气体的微生物还原作用研究进展

氧化亚氮(N₂O)是强温室气体和破坏臭氧层的主要物质之一,河湖生态系统是人为活动导致N₂O排放的热点区域.含有nosZ功能基因的N₂O还原菌(N₂ORB)是唯一已知的N₂O还原微生物,在减少N₂O排放中起着至关重要的作用.先前的研究关注于河湖中N₂O的产生和排放过程及其影响因子,缺少对N₂O汇过程及其微生物还原作用的系统报道.本研究通过系统梳理发现,寒冷的北方地区和河湖局部位点,如底泥、水库深水层和水草区,广泛表现为N₂O的汇.非反硝化N₂ORB是N₂O的净汇,新发现的nosZ Ⅱ型N₂ORB更加多样,其N₂O还原酶转位能量需求更低.相比于nosZⅠ型N₂ORB,nosZ Ⅱ型N₂ORB还原N₂O的半饱和常数更低,对N₂     

引江济太对太湖贡湖湾氧化亚氮通量的影响

选取引江济太工程中长江来水进入太湖第一站的贡湖湾为研究对象，基于2011年11月~2013年8月在贡湖湾的逐月野外调查，同时以湖心水域为参考，探讨引江济太对湖体N₂O通量的影响.结果表明，贡湖湾N₂O排放通量要显著高于湖心排放量，其N₂O通量均值分别为6.9，2.1μmol/（m²·d），但在非引水期间2个湖区的N₂O通量无显著差异.贡湖湾和湖心N₂O通量呈现明显的季节变化，且均与水温呈显著负相关关系，但因受外源来水的影响，贡湖湾N₂O通量的温度依赖程度相对较低.另外，2个湖区的N₂O通量还与营养盐等因素有关.总体上，外源引水提高了贡湖湾N₂O排放通量，但考虑到湖泊N₂O通量受到内部和外部因子的综合协同影响，外源引水对湖泊N₂O通量的具体调控机理还需要进一步探讨.     

Emissions of SO2, NO and N2O in a circulating fluidized bed combustor during co-firing coal and biomass

This paper presents the experimental investigations of the emissions of SO2, NO and N2O in a bench scale circulating fluidized bed combustor for coal combustion and co-firing coal and biomass. The thermal capacity of the combustor is 30 kW. The setup is electrically heated during startup. The influence of the excess air, the degree of the air staging, the biomass share and the feeding position of the fuels on the emissions of SO2, NO and N2O were studied. The results showed that an increase in the biomass shares resulted in an increase of the CO concentration in the flue gas, probably due to the high volatile content of the biomass. In co-firing, the emission of SO2 increased with increasing biomass share slightly, however, non-linear increase relationship between SO2 emission and fuel sulfur content was observed. Air staging significantly decreased the NO emission without raising the SO2 level. Although the change of the fuel feeding position from riser to downer resulted in a decrease in the NO emission level, no obvious change was observed for the SO2 level. Taking the coal feeding position R as a reference, the relative NO emission could significantly decrease during co-firing coal and biomass when feeding fuel at position D and keeping the first stage stoichiometry greater than 0.95. The possible mechanisms of the sulfur and nitrogen chemistry at these conditions were discussed and the ways of simultaneous reduction of SO2, NO and N2O were proposed.     

城市生活垃圾与煤流化床混烧过程中氮氧化物排放研究

针对我国城市生活垃圾热值低等特性。在流化装置上进行了城市生活垃圾与煤混燃实验，研究了在混燃过程中城市生活垃圾与煤掺烧比例及床层温度变化对NO和N2O排放浓度的影响。实验结果显示，随掺烧垃圾量逐渐增加时，NO排放浓度降低。而N2O排放浓度先降低然后增加，当城市生活垃圾与煤掺烧比例恒定时，随床温的增加NO排放浓度增加，N2O排放浓度呈下降趋势，采用前向式神经网络，以掺烧比和床温作为输入参数，对NO的排放进行预测。结果显示精度较高。     

同步硝化反硝化（SND）过程污泥聚集状态对N2O释放的影响

为实现SND高效生物脱氮及N2O减量化释放的双重目标,采用气升环流生物反应器,在实现SND高效脱氮的基础上研究了污泥的聚集状态与N2O释放特征之间的关系.采用关键酶酶促反应速率法评估了不同聚集状态污泥的硝化/反硝化活性,在相关理论分析的基础上,进行了污泥聚集状态的优化选择.结果表明,SND体系内活性污泥的聚集状态不同会...     

流化床内焦炭对N2O和NO生成和分解的影响

在小型流化床试验上进行了焦炭的燃烧试验，研究焦炭颗粒和氧化钙对Ｎ２Ｏ和ＮＯ的分解反应，焦炭颗粒对Ｎ２Ｏ还原分解速率比ＮＯ快，氧化钙对Ｎ２Ｏ分解有较强的催化作用，Ｎ２Ｏ和ＮＯ的分解反应过程可用一级Ａｒｒｈｅｎｉｕｓ公式来描述，研究不同程度脱去挥发份的炭焦颗粒对Ｎ２Ｏ和ＮＯ形成的影响，脱挥发份的程度越高，焦炭氮形成Ｎ２Ｏ的量越少，表明挥发份氮形成Ｎ２Ｏ量高于相应焦炭氮燃烧产生的Ｎ２Ｏ量，焦炭燃烧过程中     

煤粉锅炉掺烧石油焦燃烧污染物排放特性的研究

对煤粉锅炉掺烧石油焦的污染物排放特性作了较详细的研究.煤焦粉的细度对燃烧性能影响很大,因而间接地影响NO_x,SO₂排放;煤焦掺混比以及煤、焦各自的含氮、硫量对NO_x,SO₂排放影响明显;烟气中SO2的浓度随过量空气系数α的增大而减少,过量空气系数α在1.3～1.4之间时,烟气中NO_x的浓度最高.现场调试结果与实验室试验结果基本一致.实际应用中应综合考虑煤焦粉细度、煤焦掺混比以及煤焦中含氮、硫量对其燃烧特性以及NO_x,SO₂排放的影响,以确定合适的细度及煤焦掺混比投入生产运行中.      

温度对滴滤池硝化过程氧化亚氮释放的影响

研究了某大学污水处理厂的一个滴滤池(生物膜系统)随季节变化N2O的释放特征.结果表明,滴滤池中N2O的释放浓度范围为0~18.21×10-6,释放量为20.5~554g N2O/(m3?a),其释放因子(N2O-N/进水NH3-N)为0.1%~0.8%.N2O释放量与季节变化有关,夏季产生量较高而春季较少,空气和进水的温差是影响滴滤池中硝化作用和N2O释放的主要因素,7月份时气温和水温温差较小,导致空气中的氧气无法充入水中,水中溶解氧的不足使得滴滤池硝化不完全,N2O释放量最高.另外,N2O释放量的昼夜变化规律表明,滴滤池的N2O释放、硝化作用和温度变化相关,通过在线监测N2O释放和水温/气温温度变化可以间接反映滴滤池的生物硝化效果.     

Fluxes of nitric and nitrous oxides from agricultural soils in a cool temperate climate

Fluxes of NO and N₂O from sandy loam soils cropped with winter wheat and a clay loam soil under ryegrass, with and without the addition of NH₄NO₃ fertilizer, were measured using static and dynamic chamber methods. Nitric oxide fluxes ranged from −0.3 (deposition) to 6.9 (emission) ng NO-N m⁻² s⁻¹. The corresponding N₂O flux ranged from 0 to 91 (emission) ng N₂O-N m⁻² s⁻¹. The NO flux was temperature dependent. Activation energies ranged from 40 to 81 kJ mol⁻¹. Nitric oxide and N₂O fluxes increased linearly with soil available nitrogen (NH₄ + NO₃). Emissions of NO and N₂O were not detectable from unfertilized ryegrass plots. Instead, nitric oxide was absorbed by the soil and vegetation at a maximum rate of 0.31 ng NO-N m⁻² s⁻¹. The aeration state of the soil controlled the relative rates of NO and N₂O emission. Nitric oxide was the major gas emitted from well aerated soils, conditions that favour nitrification. The NO/N₂O emission ratio was >100 for the coarse-textured sandy loam soil and the clay loam soil only during low rainfall periods. Nitrous oxide was the major gas emitted from less aerated soils, conditions that allowed denitrification to occur. The NO/N₂O emission ratio was <0.001 for the clay loam soil when rainfall was high and soils were wet. Extrapolation to the U.K. situation showed that agricultural land may account for 2–6% of the total annual NO_x emission and for 16–64% of the total annual N₂O emission in the U.K.     

Catalytic reduction of nitric oxide with carbon monoxide on copper-cobalt oxides supported on nano-titanium dioxide

A series of copper-cobalt oxides supported on nano-titanium dioxide were prepared for the reduction of nitric oxide with carbon monoxide and characterized using techniques such as XRD, BET and TPR. Catalyst CuCoOx/TiO2 with Cu/Co molar ratio of 1/2, Cu- Co total loading of 30% at the calcination temperature of 350°C formed CuCo2O4 spinel and had the highest activity. NO conversion reached 98.9% at 200°C. Mechanism of the reduction was also investigated, N2O was mainly yielded below 100°C, while N2 was produced instead at higher temperature. O2 was supposed to accelerate the reaction between NOx and CO for its oxidation of NO to give more easily reduced NO2, but the oxidation of CO by O2 to CO2 decreased the speed of the reaction greatly. Either SO2 or H2O had no adverse impact on the activity of NO reduction; however, in the presence of both SO2 and H2O, the catalyst deactivated quickly.     

Effect of diet manipulation in dairy cow N balance and nitrogen oxides emissions from grasslands in northern Spain

Dietary modifications in dairy cattle have been reported as a useful strategy to alter the composition of manure. Many reports have been published on how changes in dietary crude protein content and forage-to-concentrate ratio reduces animal nitrogen (N) excretion, but little information exists about the effect of diet modification on nitrous oxide (N₂O) and nitric oxide (NO) emission when the subsequent slurry is applied on grassland. Two diets differing in forage:concentrate ratio (high forage or HF diet, 75:25; low forage or LF diet, 55:45) were tested to detect the improvement of N use efficiency in milk and the reduction of urinary and fecal N excretion. Triticale silage and barley grain were used as the main forage and concentrate sources in the diets. The subsequent slurries were characterized for N and ammonium-N content (NH₄⁺-N) and applied on grassland in order to study total and pattern of emission of N₂O and NO.The HF diet reduced the voluntary dry matter intake of the cows, N intake and urinary and fecal N excretion. However, the reduction of N intake did not improve the N use efficiency in milk (NUE) (21.0%) and did not reduce N excretion per unit of milk produced (15 g N l⁻¹) due to the lower milk yield. Slurries were similar in N content but differed in NH₄⁺ content, being lower in HF. Therefore, different slurry amounts were needed to be applied on grassland to reach the correct fertilisation rate (120 kg NH₄⁺-N ha⁻¹). Total emissions of N₂O (5.8 and 5.0 kg N₂O-N ha⁻¹) and NO (507.2 and 568.6 g NO-N ha⁻¹), and the pattern of emissions were not affected by dietary treatments. When fertilisation management depends on the collected volume to empty the slurry pit, higher N₂O and NO emissions per kg of slurry could be expected from LF slurry. Nevertheless, if slurry is applied following recommendation rates, N₂O and NO emission per unit of milk produced might be slightly lower from LF slurry. Grass yield (1.5 t dry matter ha⁻¹) and N uptake (50 kg N ha⁻¹) did not vary due to the applications of different slurries, and was attributed to low rainfalls. The correct management of the slurries on grasslands may justify an adequate nutritional strategy of dairy herds from an environmental and productive point of view.     

己二胺有机废液在流化床中焚烧的实验研究

在实验室规模的热态流化床试验台上，进行了含5％己二胺有机废液的焚烧 实验研究，在700－900℃范围内，研究温度及空气过剩系数对NOx沿床高的变化规律，以及它们对NOx排放浓度的影响。实验结果表明，沿高度方向上NOx浓度 逐渐降低，并且存在NO2浓度大于NO浓度这一有趣现象，在900℃下氧量增加有利于密相区NO、NO2浓度的降低，说明在 有氧条件下NH2促进NOx的还原，在不同空气 过剩系数下和然相区出口NOx几乎为零 ，表明900℃是己二胺有机废液焚烧 的合适温度。