2005~2017年全球大气边界层SO2时空变化

使用2005~2017年遥感数据研究了全球大气边界层SO₂时空分布特征及变化趋势.结果表明：空间分布上SO₂呈现空间异质性,大气高SO₂柱量值集中在以火山喷发为代表的自然源区域和以工业排放为代表的人为源及附近区域;一、二、三级SO₂柱量值在全球范围内整体呈现纬度地带性分布特征,北半球受人为影响较为明显,分界线在陆地区域向南凸出,海洋上向北凹陷,而南半球受人为影响较小,分界线呈现与纬线平行趋势;2005~2017年全球大气边界层SO₂单元栅格年均值整体呈现先增后减趋势,火山喷发导致2008、2009、2011年夏季出现了明显的波动,其余季节无显著变化;全球范围内大气边界层SO₂年内变化,伴随太阳直射点南北移动,2005~2014年一级SO₂柱量值延纬向对称轴的纬度,除10~12月份外,其余月份与对应月15日太阳赤纬基本吻合.     

Characteristics of volatile organic compounds, NO2, and effects on ozone formation at a site with high ozone level in Chengdu

Chengdu is a megacity in the southwest of China with high ozone (O₃) mixing ratio. Observation of volatile organic compounds (VOCs), NO₂ and O₃ with high temporal resolution was conducted in Chengdu to investigate the chemical processes and causes of high O₃ levels. The hourly mixing ratios of VOCs, NO₂, and O₃ were monitored by an online system from 28 August to 7 October, 2016. According to meteorological conditions, Chengdu, with relative warm weather and low wind speed, is favorable to O₃ formation. Part of the O₃ in Chengdu may be transported from the downtown area. In O₃ episodes, the average mixing ratios of NO₂ and O₃ were 20.20?ppbv and 47.95?ppbv, respectively. In non-O₃ episodes, the average mixing ratios of NO₂ and O₃ were 16.38?ppbv and 35.15?ppbv, respectively. The average mixing ratio of total VOCs (TVOCs) was 40.29?ppbv in non-O₃ episodes, which was lower than that in O₃ episodes (53.19?ppbv). Alkenes comprised 51.7% of the total O₃ formation potential (OFP) in Chengdu, followed by aromatics which accounted for 24.2%. Ethylene, trans-pentene, propene, and BTEX (benzene, ethylbenzene, toluene, m/p-xylene, o-xylene) were also major contributors to the OFP in Chengdu. In O₃ episodes, intensive secondary formations were observed during the campaign. Oxygenated VOCs (OVOCs), such as acetone, Methylethylketone (MEK), and Methylvinylketone (MVK) were abundant. Isoprene rapidly converted to MVK and Methacrolein (MACR) during O₃ episodes. Acetone was mainly the oxidant of C3-C5 hydrocarbons.     

Morphology and composition of particles emitted from a port fuel injection gasoline vehicle under real-world driving test cycles

Traffic vehicles, many of which are powered by port fuel injection (PFI) engines, are major sources of particulate matter in the urban atmosphere. We studied particles from the emission of a commercial PFI-engine vehicle when it was running under the states of cold start, hot start, hot stabilized running, idle and acceleration, using a transmission electron microscope and an energy-dispersive X-ray detector. Results showed that the particles were mainly composed of organic, soot, and Ca-rich particles, with a small amount of S-rich and metal-containing particles, and displayed a unimodal size distribution with the peak at 600?nm. The emissions were highest under the cold start running state, followed by the hot start, hot stabilized, acceleration, and idle running states. Organic particles under the hot start and hot stabilized running states were higher than those of other running states. Soot particles were highest under the cold start running state. Under the idle running state, the relative number fraction of Ca-rich particles was high although their absolute number was low. These results indicate that PFI-engine vehicles emit substantial primary particles, which favor the formation of secondary aerosols via providing reaction sites and reaction catalysts, as well as supplying soot, organic, mineral and metal particles in the size range of the accumulation mode. In addition, the contents of Ca, P, and Zn in organic particles may serve as fingerprints for source apportionment of particles from PFI-engine vehicles.     

Visible-light-driven photocatalytic inactivation of bacteriophage f2 by Cu-TiO2 nanofibers in the presence of humic acid

Pathogenic viruses in drinking water are great threats to public health. Visible-light-driven photocatalysis is a promising technology for virus inactivation. However, the existing photocatalytic antiviral research studies have mostly been carried out in single-component systems, neglecting the effect of natural organic matter, which exists widely in actual water bodies. In this paper, electrospun Cu-TiO₂ nanofibers were prepared as photocatalysts, and their photocatalytic antiviral performance in the presence of humic acid (HA) was comprehensively studied for the first time. The properties of the reaction mixture were measured during the reaction. In addition, the safety, reliability and stability of photocatalytic disinfection in the mixed system were evaluated. The results showed that the virus removal efficiency decreased with the increase of the HA concentration. The type of reaction solution, such as PBS buffer solution or water, did not affect the removal efficiency noticeably. Under acidic conditions, the electrostatic forces between photocatalysts and viruses were strengthened, leading to higher virus removal efficiency. As the reaction time went on, the pH value in the solution increased first and then tended to be stable, the conductivity remained stable, and the dissolved oxygen increased first and then decreased. The safety test showed that the concentration of Cu ions released into the solution was lower than specified by the international standards. No photoreactivation was observed, and the addition of HA significantly reduced the reutilization efficiency of the photocatalysts.     

Three-dimensional biogenic C-doped Bi2MoO6/In2O3-ZnO Z-scheme heterojunctions derived from a layered precursor

Novel 3D biogenic C-doped Bi_2 MoO_6/In_2O_3-ZnO Z-scheme heterojunctions were synthesized for the first time, using cotton fiber as template. The as-prepared samples showed excellent adsorption and photodegradation performance toward the hazardous antibiotic doxycycline under simulated sunlight irradiation. The morphology, phase composition and in situ carbon doping could be precisely controlled by adjusting processing parameters. The carbon doping in Bi_2 MoO_6/In_2O_3-ZnO was derived from the cotton template, and the carbon content could be varied in the range 0.9–4.4 wt.% via controlling the heat treatment temperature. The sample with Bi_2 MoO_6/In_2O_3-ZnO molar ratio of 1:2 and carbon content of1.1 wt.% exhibited the highest photocatalytic activity toward doxycycline degradation,which was 3.6 and 4.3 times higher than those of pure Bi_2 MoO_6 and Zn In Al-CLDH(calcined layered double hydroxides), respectively. It is believed that the Z-scheme heterojunction with C-doping, the 3D hierarchically micro–meso–macro porous structure, as well as the high adsorption capacity, contributed significantly to the enhanced photocatalytic activity.     

水泥-电力行业的产业共生网络构建及区域案例研究

水泥工业作为工业生态系统的汇,能够多样化地利用其他行业的副产物,这种典型的产业共生模式可以通过减少资源和能源的消耗带来显著的CO₂减排效果.由于产业共生在水泥行业具有一定的普遍性及巨大的CO₂减排潜力,所以对水泥工业产业共生现状的了解与分析就显得尤为重要;而通过对产业共生现状的全面了解,才能对现有水泥行业产业共生的程度进行分析,并以此为参照,对未来不同政策与情景下的CO₂减排潜力进行量化与评估.为实现对产业共生实际情况的模拟,以水泥-电力行业的产业共生为例,采用最优化的方法,提出了一套基于一般统计数据来模拟产业共生实际情况的系统方法,将技术、经济与政策3类不同的决策变量影响纳入模型,以模拟出最接近真实情景的产业共生情况.为验证模型的有效性,对新乡市水泥-电力行业实际的产业共生情况进行分析.结果表明:新乡市水泥-电力行业间存在普遍的产业共生现象,实地调查中有77.8%（21家）的水泥制造企业利用粉煤灰作为水泥制造的原材料.将一般统计数据与实地调查数据对比发现,一般统计数据能较好地反映企业实际物质投入产出情况;利用一般统计数据,模型对新乡市产业共生网络结构模拟的准确率高达92.6%,显示该模型能较为有效地对产业共生的实际情况进行模拟.      

乌鲁木齐市散煤燃烧大气污染物排放清单及时空分布特征

为研究乌鲁木齐市散煤燃烧对大气污染物的贡献情况,根据实地调研收集到的散煤燃烧活动水平数据,利用排放因子法建立2015年乌鲁木齐市散煤燃烧PM_2.5、SO₂和NO_x的排放清单,利用ArcGIS空间分析工具进行空间分布特征分析,使用蒙特卡罗方法进行不确定性分析.结果表明:2015年散煤燃烧排放PM_2.5、SO₂、NO_x分别为1.70×104、4.13×104、2.80×103 t.PM_2.5和SO₂排放的主要贡献区域为乌鲁木齐县,分别占排放总量的27.35%和26.23%,这是由于乌鲁木齐县社区居民和大棚种植耗煤量较大所致;NO_x排放的主要贡献区域为米东区,贡献率高达28.03%,这是因为米东区社区居民所用炉灶为手动炉排层燃炉灶,其排放因子较大所致.空间分布特征表明,污染物主要分布在米东区南部、沙依巴克区北部及乌鲁木齐县中部.不确定性分析表明,村庄、社区、大棚种植、商业和事业单位在95%的置信区间时不确定性分别为-69%~165%、-57%~116%、-68%~171%和-67%~165%.蒙特卡罗预测结果（平均值）高于排放清单的计算结果.研究显示,乌鲁木齐市散煤燃烧对污染物排放贡献较大,并且具有明显的季节性和区域性特征.      

CO2倍增和施氮对水稻不同生长期土壤反硝化细菌丰度的影响

随着全球气候变化的不断加剧,大气CO₂浓度呈明显增加趋势,这将间接影响土壤-植物-微生物系统的氮循环过程.为研究典型水稻土壤反硝化细菌对CO₂浓度升高的响应规律和机制,借助水稻密闭培养箱,运用实时荧光定量聚合酶链式反应（Real-Time qPCR）分子技术,设置不施氮（0 mg/kg）和常规施氮（100 mg/kg）2个处理,研究CO₂倍增对水稻不同生长期土壤关键反硝化功能细菌（narG、nirK和nirS型）丰度的影响.结果表明:①在2种施氮水平,CO₂倍增显著促进了水稻分蘖期、孕穗期、扬花期和成熟期水稻根系生长（增幅为2.96%~28.4%）、地上部生物量增加（增幅为7.1%~107.3%）以及成熟期籽粒干质量的增加（增幅为19.5%和38.0%）,具有显著的增产效应.②反硝化细菌丰度对CO₂倍增的响应与生育期及施氮水平有关,CO₂倍增在2个施氮水平均抑制分蘖期反硝化细菌的繁殖,显著增加孕穗期反硝化细菌数量;在水稻扬花期,CO₂倍增促进了施氮处理narG和nirS型反硝化细菌数量的增加,在成熟期抑制未施氮处理下narG、nirK和nirS型反硝化细菌的生长.另外,narG、nirK、nirS型反硝化细菌丰度整体表现为narG > nirS > nirK,且随水稻的生长,其在成熟期的丰度均呈降低趋势.nirK和nirS基因同属亚硝酸还原酶,但nirS基因丰度高于nirK,且对CO₂倍增和施氮的响应有所差异.研究显示,CO₂倍增可显著增加水稻生长和产量,不同施氮水平对稻田土壤反硝化细菌丰度的影响存在差异.      

兰州市典型企业VOCs排放特征及反应活性分析

基于兰州市大气VOCs排放清单,选取石化厂、乙烯厂、涂料厂3个典型企业采集VOCs样品,分析其无组织排放特征,并采用MIR（最大增量反应活性）法和LOH（·OH反应速率）法综合评价其化学反应活性,识别各企业的VOCs活性优势物种,同时探究不同企业特征VOCs比值.结果表明:不同排放源φ（VOCs）差异较大,范围为20.8×10-9~6 520.3×10-9.从VOCs物种构成上来看,涂料厂芳香烃占比最高,而石化厂、乙烯厂均以烷烃物种最为丰富,石化厂不同工艺VOCs物种构成略有差异.从活性上看,涂料厂VOCs活性最高,其LOH和OFP（臭氧生成潜势）分别为2 676.9 s-1和72 519.0×10-9,约为其他行业的18~1 000倍,间/对-二甲苯、乙苯、邻二甲苯等物种活性较大;其次为石化厂,其LOH和OFP分别为273.2 s-1和4 039.1×10-9,正戊烷、异戊烷、乙烯、丙烯等物种活性贡献率高,其中柴油工艺对石化厂VOCs活性贡献率最大;乙烯厂的OFP最低,其LOH和OFP分别为4.6 s-1和69.7×10-9,其VOCs活性主要来自乙烯、丙烯、正丁烯等烯烃物种.各工业源BTEX（苯、甲苯、乙苯及3种二甲苯异构体的合称）分布具有一定的差异,对于指示不同VOCs来源有一定的参考价值,但不同源比值的重叠性也表明并非全部VOCs来源可以通过特征物种比值来区分.研究显示,控制工业源特别是涂料与石化工业VOCs的排放有助于控制兰州市O₃的生成.      

中国超大城市碳排放达峰的影响因素及组合情景预测——基于门限-STIRPAT模型的研究

城市是中国碳排放的重要来源,而超大城市的碳达峰研究对国内其他城市和全国能否实现碳达峰目标具有重要的现实意义.以北京、上海、广州、深圳、天津和重庆等6个超大城市为研究对象,能源强度为门限变量,建立门限-STIRPAT模型,首先确定6个超大城市碳排放的驱动因素,然后对27种情景下的各城市碳排放达峰进行预测.研究结果表明:①人口、人均GDP和能源强度对各城市碳排放起到正向促进效应,人口的影响效应最大,其次是能源强度,人均GDP对碳排放的影响最小.②能源强度对二氧化碳排放的影响呈阶段性变化特征.③北京、上海和重庆在高能源强度下降率的情景下,已经达峰;天津、除最宽松的高-高-高情景外的广州和深圳会在2030年前实现达峰.如果能源强度以中速率下降,6个城市碳排放不能保证一定能在2030年前达峰.如果能源强度以低速率下降,6个城市均不能在2030年前达峰.本研究有利于明确超大城市碳排放的影响因素,对其他城市尽快实现碳排放达峰具有借鉴意义,为全国实现碳达峰目标提供可行的研究思路.