Removal of NOx from flue gas with radical oxidation combined with chemical scrubber

In this paper, removal of NOx(namely DeNOx) from flue gas by radical injection combined with NaOH solution(26% by weight of NaOH in water) scrubbing was investigated. The experimental results showed that the steady streamer corona occurs through adjusting the flow rate of the oxygen fed into the nozzles electrode. The vapor in the oxygen has influence on the V-I characteristics of corona discharge. Both HNO2 and HNO3 come into being in the plasma reactor and the DeNOx efficiency in the plasma reactor is more than 60%. The overall DeNOx efficiency of the whole system reaches 81.7 % when the NaOH solution scrubbing is collaborated.     

Determination of hydroxyl radicals with salicylic acid in aqueous nitrate and nitrite solutions

The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicylic acid was employed as an innovative molecular probe of hydroxyl radical(OH) generated in aqueous nitrate and nitrite solutions through photochemical reactions. Kinetic studies showed that the steady-state concentrations of OH in aqueous NO3^-(10 mmol/L, pH=5) and NO2^ (10 mmol/L, pH=5) solutions under ultraviolet irradiation were at a same magnitude, 10v-15 mol/L. Apparent quantum yields of OH at 313 nm were measured as 0.011 and 0.07 for NO3^- and NO2^ respectively, all comparable to the results of previous studies.     

臭氧氧化分解饮用水中嗅味物质2-甲基异莰醇

比较了几种常见氧化剂对饮用水中嗅味物质2-甲基异莰醇(2-methylisoborneol,MIB)的氧化去除效果.结果表明,KMnO₄、NaClO、H₂O₂等氧化剂的氧化作用对水中MIB的去除效果均较差,而臭氧却能有效地将其氧化;考察了pH对臭氧化去除MIB的影响规律,发现pH在7.0～10.0条件下,随着pH值增加MIB去除率增加,但当pH达到10.0左右时,MIB的去除率反而下降;MIB的臭氧化去除效果随着自由基捕获剂(重碳酸盐和叔丁醇)的浓度增加而明显地降低,说明臭氧化去除水中MIB主要遵循自由基作用机理;以松花江江水为本底进行试验和与蒸馏水进行试验的结果相差不大,原因可能是由于松花江水体中碳酸盐浓度较低(小于50 mg/L),对自由基捕获能力较小,同时江水中的部分腐殖质(NOM)对臭氧去除MIB的过程起到了促进作用.     

光催化氧化/吸收工艺处理垃圾焚烧发电厂恶臭废气

我国南方某城市垃圾焚烧发电厂采用光催化氧化技术/吸收工艺联用技术对难降解恶臭气体进行高效处理,大大提高了恶臭气体的去除效率,实现了该行业废气的无害化处理,取得了良好的效果。运行结果显示,光催化氧化技术/吸收工艺联用技术能实现难降解恶臭气体的高效处理,排放废气可达到《恶臭污染物排放标准》(GB14554-93)中的二级标准。     

典型工业城市夏季VOCs污染特征及反应活性

为研究典型工业城市夏季挥发性有机物（VOCs）污染对环境的影响及成因,利用2020年7月在淄博市城区的VOCs在线监测数据,分析了污染日和清洁日VOCs的污染特征、化学反应活性和臭氧（O₃）污染成因.结果表明,污染日总挥发性有机物（TVOC）小时浓度均值较清洁日高32.5%,分别为（50.6±28.3）μg·m^-3和（38.2±24.9）μg·m^-3,污染日和清洁日各组分贡献率均为：烷烃>芳香烃>烯烃>炔烃,TVOC和O₃浓度日变化均呈现相反的变化趋势.污染日臭氧生成潜势（OFP）、·OH消耗速率（L_·OH）和二次有机气溶胶生成潜势（SOA_p）均高于清洁日,烯烃对OFP和L_·OH贡献最大,芳香烃对SOA_p贡献最大;OFP和SOA_p日变化趋势和TVOC基本一致;化学反应活性优势物种以烯烃和芳香烃类物质居多.VOCs/NO_x法判断污染日和清洁日O₃敏感区属性均处于VOCs控制区和过渡区,而烟雾产量模型法（SPM）诊断污染日O₃敏感区属性在08：00~16：00期间处于VOCs控制区和过渡区交替状态,清洁日各时段均处于VOCs控制区.为减轻该市夏季O₃污染,应加强对VOCs （烯烃和芳香烃）和氮氧化物（NO_x）的协同控制.     

连续测量大气·OH的化学电离飞行时间质谱仪的研制

搭建了一套化学电离飞行时间质谱仪用于连续测量大气·OH.该仪器采用了基于63Ni放射源的双管正交式结构大气压化学电离源电离大气中的·OH,最大程度地避免了试剂气体电离及滴定、转化反应间的相互干扰.63Ni放射源首先电离HNO3试剂气体得到试剂离子NO-3,·OH在反应管中与SO2反应最终转化为H2SO4,NO-3与H2SO4发生化学电离反应生成HSO-4离子,进入到质谱仪中进行检测,通过测量NO-3与HSO-4离子的强度,利用化学电离反应方程可直接计算出大气中OH的浓度.所研制仪器用于实验室内·OH的在线检测,在5 s内测得·OH的浓度为1.6×106个·cm-3,实验结果显示该仪器可用于原位连续测量大气中的超痕量自由基.     

Selected dark sides of biomass-derived biochars as environmental amendments

With the rapid increase in the application of biochars as amendments, studies are needed to clarify the possible environmental risks derived from biochars to use safely the biomass resources. This work reported selected dark sides of maize straw-and swine manurederived biochars pyrolyzed at 300 and 500°C. During the pyrolysis processes, total heavy metals in the biochars were enriched greatly accompanying with considerable emission of the heavy metals into atmosphere and the trends became increasingly obvious with pyrolysis temperature. Meanwhile, the biochars showed distinctly decreased available heavy metals compared with raw feedstocks, which could be mainly attributed to the sorption by the inorganics in the biochars. The water-and acid-washing treatments significantly increased the releasing risks of heavy metals from biochars into the environments. Electron paramagnetic resonance analysis indicated that persistent free radicals, emerged strongly in the biochars as a function of the aromatization of biomass feedstocks, were free from the influence of water-, acid-, or organic-washing of the biochars and could remain stable even after aged in soils for 30 days. Dissolved biochars, highly produced during pyrolysis processes, showed distinct properties including lower molecular weight distribution while higher aromaticity compared with soil dissolved organic carbon.The results of this study provide important perspectives on the safe usage of biochars as agricultural/environmental amendments.     

Enhancement of municipal sludge dewaterability by electrochemical pretreatment

Electrolysis is a promising technology to improve sludge dewaterability efficiently with negligible environmental impact. To intensify the electrolytic efficiency, the effect of electrolytes (NaCl, Na₂SO₄, NaNO₃, and NaClO₄) on electrolysis pretreatment of municipal sludge and its mechanisms was investigated using Ti/PbO₂ electrodes. The electrolytes, which enhanced the production of oxidative radicals, showed a significant synergetic effect in reducing the capillary suction time (CST) of sludge. NaCl was distinguished from the other electrolytes since it formed a large amount of active chlorine species, which oxidized the sludge cells to improve the sludge dewaterability. The surface morphologies as well as the soluble proteins and polysaccharides were analyzed to unravel the underlying mechanisms of sludge dewaterability. Additionally, an economic assessment showed that NaCl addition in the electrolysis pretreatment can be a suitable technique for enhancing municipal sludge dewaterability.     

铁酸铜非均相活化过硫酸盐降解罗丹明B

采用新型磁性催化材料尖晶石型铁酸铜（CuFe₂O₄）活化过硫酸盐（PMS）降解氧杂蒽类染料罗丹明B（RhB）,考察PMS浓度、CuFe₂O₄投加量、pH值和水中常见离子对RhB降解的影响.结果表明,当RhB、PMS、CuFe₂O₄初始浓度分别为5 μmol/L、0.1mmol/L、0.1g/L时,在中性条件下反应30min后RhB去除率可达88.87%.其中,Cl^-和HCO₃^-对RhB的降解无显著影响,而H₂PO₄^2-、C₂O₄^2-及腐殖酸明显抑制RhB的降解.自由基鉴定实验表明,在中性及弱碱性条件下SO₄^-和·OH是CuFe₂O₄/PMS体系降解RhB的主要自由基.研究发现随着RhB的降解,溶液逐渐褪色并伴随着甲酸根、乙酸根、草酸根和铵根离子的生成,原因在于SO₄^-和·OH可以破坏RhB分子的发色基团,使苯环开环和氮原子脱落,形成相应的降解产物.矿化实验表明0.2mmol/L的RhB在CuFe₂O₄/PMS体系中反应10h后,矿化率可达62%.催化剂的重复利用实验表明制备的CuFe₂O₄具有良好回收再利用能力.     

挥发性有机物(VOCs)的不同化学去除途径:城市与区域站点的对比

VOCs在大气中主要是与OH自由基、NO₃自由基和O₃等反应氧化去除,部分OVOCs的自身光解也是重要的化学去除途径.本研究基于2018年和2019年秋季在珠三角地区的城市和区域站点的外场观测实验,使用VOCs、常规痕量气体及气象参数的观测数据,对烷烃、烯烃、芳香烃和OVOCs等VOCs组分不同化学去除途径的去除速率进行分析.结果表明,烷烃和芳香烃主要通过与OH自由基反应去除,最高占比超过99%.与NO₃自由基和O₃的反应可贡献烯烃去除速率的80%以上,特别是一些天然源的烯烃（如单萜烯）与NO₃自由基的氧化去除是贡献最大的氧化途径.光解是甲醛最重要的去除途径,在两个站点均达到了50%以上,酮类的光解贡献会高于其他OVOCs类物质.OH自由基的氧化去除途径在城市和区域站点的人为源及天然源VOCs去除中占主导地位.区域站点,烯烃尤其是天然源的烯烃物种,与NO₃自由基和O₃反应的贡献要高于城市站点.本研究对促进不同VOCs物种在大气中的去除途径以及其空间差异的认识有重要意义.