北京南部城区PM2.5中碳质组分特征

为了解《大气污染防治行动计划》实施后北京市大气PM_2.5中碳质组分特征,于2017年12月至2018年12月在北京污染较重的南部城区进行了PM_2.5连续采样,对其中的有机碳（OC）和元素碳（EC）进行了全面研究.结果表明,北京大气PM_2.5、OC和EC浓度变化范围分别为4.2~366.3、0.9~74.5和0.0~5.5 μg ·m^-3,平均浓度分别为（77.1±52.1）、（11.2±7.8）和（1.2±0.8）μg ·m^-3,碳质组分（OC和EC）整体占PM_2.5的16.1%.OC质量浓度季节特征表现为：冬季[（13.8±8.7）μg ·m^-3] > 春季[（12.7±9.6）μg ·m^-3] > 秋季[（11.8±6.2）μg ·m^-3] > 夏季[（6.5±2.1）μg ·m^-3],EC四季质量浓度水平均较低,范围为0.8~1.5 μg ·m^-3.二次有机碳（SOC）年均质量浓度为（5.4±5.8）μg ·m^-3,四季贡献比例范围为45.7%~52.3%,年均贡献为48.2%,凸显了二次形成的重要贡献.随污染加重,尽管OC和EC贡献比例均降低,但浓度水平却成倍升高,OC和EC浓度在严重污染天分别是空气质量为优天的6.3和3.2倍.与非供暖时段相比,供暖时段PM_2.5、OC和SOC浓度分别增加了14.4%、47.9%和72.1%,体现了OC对供暖季PM_2.5污染的重要贡献.PSCF分析表明,位于北京西南的山西省和河南省部分区域是PM_2.5和OC的主要潜在源区,且PM_2.5潜在源区更为集中;EC的PSCF高值（>0.7）区域较少,主要位于北京南部,如山东省和河南省部分地区,且北京市及周边地区贡献明显.     

铝系混凝剂优势形态分析及其混凝特性

聚合氯化铝（PACl）是常用的水处理混凝剂,在应用过程中通常表现出比传统铝盐更为优异的效果.研究表明,这种优异性能主要得益于其特殊的组成,特别是高分子聚合物Al₁₃和Al₃₀独特的物化特性.Al₁₃和Al₃₀是铝离子水解过程中的中间产物,在地球科学和环境化学等领域有着重要的研究价值.于水处理而言,二者的结构和分子特性是研究者关注的重点,大量研究基于此展开,很多重要的发现为实际应用奠定了基础.基于对PACl及其组成性质的研究,本文对PACl的混凝特性及其优势形态分子的分析进行了综合阐述.     

固定化微藻流化床反应器去除低碳污水中氨氮的潜力

以固定化微藻颗粒为原料,通过搭建流化床反应器强化微藻对氨氮（NH₄⁺-N）的去除,设计了藻种、污水上升流速、光周期和光照强度四组单一变量实验,系统地研究了不同条件下微藻去除NH₄⁺-N的能力.结果表明,当以固定化斜生栅藻为原料、污水上升流速为6.8m/h、光周期为8：16h和光照强度为4800Lux时,NH₄⁺-N去除效果最优（96.7%）.在最优操作条件下,探究了COD为200mg/L时微藻去除NH₄⁺-N的潜力,结果表明,当NH₄⁺-N初始浓度不高于50mg/L时,NH₄⁺-N去除率高于95%.本实验建立了一套半连续微藻流化床实验方法,该方法显著减弱了微藻在生物同化过程中对有机碳源的依赖性,为低COD条件下微藻生物脱氮工艺的设计提供了技术参考和理论基础.     

黄海麻坑群沉积物磷的保存与转化及环境效应

基于对北黄海典型麻坑群海域某单位麻坑内部和外缘沉积物中不同赋存形态的磷、甲烷（CH₄）和硫化物等参数的分析,探讨了麻坑独特的环境中磷的转化与埋藏机制、沉积物-水体系磷的释放及对区域磷循环的影响.研究表明,沉积物中碎屑态磷（Det-P）是磷主要的赋存形态（>50%）,其次是有机磷（Org-P）、铁结合态磷（Fe-P）和自生态磷（Auth-P）,交换态磷（Exch-P）对总磷的贡献较小;麻坑内部与麻坑外缘处沉积物中溶解态活性磷（DRP）向水体的释放通量分别为2.84μmol/（cm²·a）和1.03μmol/（cm²·a）,对上层水体的贡献依次为19.6%和3.03%,是上层水体磷的重要来源.麻坑内外磷的埋藏速率与转化过程存在不同;研究区地下水的渗漏是磷的沉积速率和释放通量都普遍高的原因.北黄海麻坑区沉积物中磷的保存与转化还与浅层CH₄的逸出相关,潜在提高黄铁矿的生成速率.较高的沉积物-水界面磷通量必然对区域富营养化等生态环境问题产生深远影响,值得关注.     

黄土高原人工刺槐林土壤团聚体中不同活性有机碳从南到北的变化特征

不同粒径团聚体中的不同活性有机碳对人工林土壤质量改善及碳库动态平衡有重要的作用.本研究在黄土高原地区,从南向北沿着降雨和温度降低梯度选择淳化、安塞、绥德和神木共4个地区,比较研究了人工刺槐林土壤团聚体不同的活性有机碳含量变化及其影响因素.通过湿筛法将土壤团聚体分级为粉黏粒（<0.053 mm）、微团聚体（0.25~0.053 mm）和大团聚体（>0.25 mm）,用Leffory法测定3种粒径土壤团聚体低、中、高活性有机碳含量.结果表明：①4个样区大团聚体（>0.25 mm）含量由南至北呈先降低后增加趋势,微团聚体（0.25~0.053 mm）含量逐渐增加,粉黏粒（<0.053 mm）含量则先增后减.②4个样区中土壤团聚体3种活性有机碳含量大小顺序为低活性 > 中活性 > 高活性,其中,粉黏粒（<0.053 mm）低活性有机碳含量为1.02~1.52 g·kg^-1,中活性有机碳含量为0.53~0.91 g·kg^-1,高活性有机碳含量为0.28~0.43 g·kg^-1;而微团聚体（0.25~0.053 mm）低活性有机碳含量为1.02~2.02 g·kg^-1,中活性有机碳含量为0.46~1.20 g·kg^-1,高活性有机碳含量为0.31~0.85 g·kg^-1;大团聚体（>0.25 mm）低活性有机碳含量为1.08~3.07 g·kg^-1,中活性有机碳含量为0.70~1.96 g·kg^-1,高活性有机碳含量为0.48~1.24 g·kg^-1.③黄土高原人工刺槐林3种粒径团聚体的低、中、高活性有机碳含量主要与年均气温（MAT）、年均降雨量（MAP）、土壤SOC、TN和含水率显著相关（p<0.05）,且在同一活性下,活性有机碳含量与MAT、MAP、土壤TN、SOC、含水率的相关性随着土壤团聚体粒径的增大而越显著.研究结果对理解黄土高原土壤团聚体活性有机碳含量在空间尺度上的变化特征和影响因素具有重要意义.     

Ca(OH)2解吸并固定混合吸收液中CO2的实验研究

CO₂化学吸收法分离纯度高,技术成熟,但能耗过高及成本是困扰该技术发展的瓶颈.在常压条件下对利用Ca（OH）₂直接矿物碳酸化固定MDEA/PZ混合吸收富液中CO₂进行了一系列实验研究,考察了吸收液负荷、Ca（OH）₂投加量、pH、温度及搅拌速率等因素对解吸率的影响,并利用动态吸收-解吸循环实验研究了其CO₂吸收性能和循环使用稳定性,最后对碳酸化反应产物进行了XRD、TEM分析.结果表明,在常压条件下,Ca（OH）₂可以通过液相直接矿物碳酸化对CO₂进行直接固定,并实现吸收富液的再生;随着负荷的升高及Ca（OH）₂投加量、pH、搅拌速率的增大,解吸率随之增加;随着溶液温度升高,解吸率下降;经过5次动态吸收-解吸循环实验后CO₂吸收量可以达到并保持在0.57 mol·L^-1,显示出了良好的循环稳定性.     

Cytotoxicity of the soluble and insoluble fractions of atmospheric fine particulate matter

Inhaled atmospheric fine particulate matter(PM_(2.5)) includes soluble and insoluble fractions,and each fraction can interact with cells and cause adverse effects.PM_(2.5) samples were collected in Jinan,China,and the soluble and insoluble fractions were separated.According to physiochemical characterization,the soluble fraction mainly contains watersoluble ions and organic acids,and the insoluble fraction mainly contains kaolinite,calcium carbonate and some organic carbon.The interaction between PM_(2.5) and model cell membranes was examined with a quartz crystal microbalance with dissipation(QCM-D) to quantify PM_(2.5) attachment on membranes and membrane disruption.The cytotoxicity of the total PM_(2.5) and the soluble and insoluble fractions,was investigated.Negatively charged PM_(2.5) can adhere to the positively charged membranes and disrupt them.PM_(2.5)also adheres to negatively charged membranes but does not cause membrane rupture.Therefore,electrostatic repulsion does not prevent PM_(2.5) attachment,but electrostatic attraction induces remarkable membrane rupture.The human lung epithelial cell line A549 was used for cytotoxicity assessment.The detected membrane leakage,cellular swelling and blebbing indicated a cell necrosis process.Moreover,the insoluble PM_(2.5) fraction caused a higher cell mortality and more serious cell membrane damage than the soluble fraction.The levels of reactive oxygen species(ROS) enhanced by the two fractions were not significantly different.The findings provide more information to better understand the mechanism of PM_(2.5) cytotoxicity and the effect of PM_(2.5) solubility on cytotoxicity.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

Coupling mechanism of activated carbon mixed with dust for flue gas desulfurization and denitrification

To clarify the effect of coking dust, sintering dust and fly ash on the activity of activated carbon for various industrial flue gas desulfurization and denitrification, the coupling mechanism of the mixed activated carbon and dust was investigated to provide theoretical reference for the stable operation. The results show that coking dust had 34% desulfurization efficiency and 10% denitrification efficiency; correspondingly, sintering dust and fly ash had no obvious desulfurization and denitrification activities. For the mixture of activated carbon and dust, the coking dust reduced the desulfurization and denitrification efficiencies by blocking the pores of activated carbon, and its inhibiting effect on activated carbon was larger than its own desulfurization and denitrification activity. The sintering dust also reduced the desulfurization efficiency on the activated carbon while enhancing the denitrification efficiency. Fly ash blocked the pores of activated carbon and reduced its reaction activity. The reaction activity of coking dust mainly came from the surface functional groups, similar to that of activated carbon. The reaction activity of sintering dust mainly came from the oxidative property of Fe₂O₃, which oxidized NO to NO₂ and promoted the fast selectively catalytic reduction (SCR) of NO to form N₂. Sintering dust was activated by the joint action of activated carbon, and both had a coupling function. Sintering dust enhanced the adsorption and oxidation of NO, and activated carbon further promoted the reduction of NO_x by NH₃; thus, the denitrification efficiency increased by 5%-7% on the activated carbon.     

餐厨垃圾生物有机肥对贫瘠黄褐土改良的研究

为了阐明餐厨垃圾生物有机肥改良贫瘠土壤的作用机制,以贫瘠黄褐土为研究对象,通过不施肥、长期（>5 a）施用化肥、中长期（5 a）施用少量餐厨垃圾生物有机肥和短期（1 a）施用大量餐厨垃圾生物有机肥4种施肥方式,分别记为CK组、CF组、LOF-5组和MOF-1组,对比分析不同施肥方式对土壤OM（有机质）、活性有机碳、营养元素和团聚体等的影响.结果表明:①施用餐厨垃圾生物有机肥可显著提高土壤OM、活性有机碳含量,其中,MOF-1组提高效果最显著,与CK组相比,w（OM）可提高173.29%,w（ROC）（ROC为易氧化有机碳）增加了39.17%,w（POC）（POC为颗粒有机碳）和w（DOC）（DOC为可溶性有机碳）分别是CK组的13.85和10.32倍.②中长期（5 a）施用少量餐厨垃圾生物有机肥可增加土壤中较大粒径团聚体的占比,且更有利于提高土壤团粒结构的稳定性,LOF-5组>2 mm粒级的团聚体占比是CK组的4.68倍;与CK组相比,LOF-5组MWD（平均重量直径）增加了100.00%,GMD（几何平均直径）增加了82.98%,>0.25 mm水稳定性团聚体质量占比（DR_0.25）增加了27.20%.③中长期（5 a）施用少量餐厨垃圾生物有机肥可增加土壤中w（TN）（TN为全氮）和w（AN）（AN为速效氮）,与CK组相比,LOF-5组w（TN）和w（AN）分别增加了77.42%和20.82%.施用餐厨垃圾有机肥也可同时增加土壤中w（AP）（AP为速效磷）和w（AK）（AK为速效钾）,MOF-1组增加效果较佳,w（AP）和w（AK）分别是CK组的9.43和3.39倍.研究显示,中长期（5 a）施用少量餐厨垃圾生物有机肥可提升土壤固碳能力,提高土壤养分利用的有效性,从而提升耕地土壤质量,减少化肥施用量,是我国贫瘠黄褐土改良的有效施肥模式.