低NOx环境异戊二烯促进甲苯生成甲基丁烯二醛的模拟实验

在低NO_x浓度条件下开展甲苯和异戊二烯复合体系的烟雾箱模拟实验,使用高时间分辨率的在线质子转移反应飞行时间质谱(PTR-TOF-MS)实时监测混合体系中反应物与产物的浓度变化情况,探究人为源与天然源交汇过程中, 自然源挥发性有机物 (BVOCs)对人为挥发性有机物(AVOCs)化学降解的影响.结果表明,异戊二烯与甲苯竞争OH自由基,从而抑制了甲苯的化学降解,该竞争反应开始得越早,抑制效果越显著.研究还发现异戊二烯会增强甲苯RO₂降解途径产物的产量,生成更多1,4不饱和-二羰基化合物(如丁烯二醛和甲基丁烯二醛)与二羰基化合物(如乙二醛和甲基乙二醛),其中甲基丁烯二醛增量最高可达38.6%.此外,异戊二烯快速氧化生成的RO₂自由基碳数更少,可能与甲苯氧化生成的RO₂自由基发生了快速的交叉反应,有利于甲苯RO自由基的生成及裂解,最终导致甲苯RO₂途径裂解产物的增加.     

正渗透去除地表水中DOM的效能研究

采用经砂滤处理后的滆湖水作为原料液,氯化钠溶液作为汲取液,在不同影响因素条件下进行正渗透试验,并对试验后的膜片进行清洗,探究膜污染的可逆性.结果表明:提高汲取液浓度、运行温度及膜面流速均可有效增加膜通量;正渗透对滆湖水体中的溶解性微生物代谢产物、类色氨酸、类富里酸和腐殖酸四种主要DOM成分均有较好的去除效果,DOC、UV₂₅₄截留率均在96%以上;短期运行通过水力清洗几乎可以完全恢复膜通量,而长期运行通过超声清洗可以基本恢复全部膜通量,通过分析膜清洗液可知造成膜污染的主要物质为类色氨酸类和类富里酸类物质.     

天津市减污降碳协同效应评估与预测

为评估和预测天津市减污降碳协同效应,采用减排量弹性系数法评估减污降碳协同效应,基于STIRPAT模型预测天津市“十四五”期间的减污降碳协同效应,并分情景预测天津市2026~2060年的减污降碳协同效应.结果表明：大气污染当量和温室气体的主要排放源均为工业源;2015~2017年天津市减污降碳协同效应系数范围为0.11~0.26,2013~2014年和2018~2020年天津市的减污降碳协同效应系数均小于0;天津市“十四五”期间减污降碳协同效应系数为0.06;各种情景下,2026~2060年天津市减污降碳协同效应系数均大于0.天津市2011~2020年减污降碳协同效应波动变化,“十四五”时期或可进入减污降碳协同增效阶段.天津市要在2026~2060年实现较高水平的减污降碳协同增效,就需要合理控制城镇化率、人口总数和地区生产总值,增加第三产业比重和高技术比重,持续降低能源强度.     

成渝城市群碳排放时空特征及其影响因素

利用2008~2018年成渝城市群内16个城市的面板数据,运用空间自相关和时空地理加权回归模型,探究了城市群碳排放的时空演变格局,揭示了碳排放影响因素的时空异质性.结果表明,成渝城市群碳排放整体呈增长态势,总量由5亿t增加到6.6亿t,增速约为1500t/a,地均碳排放量和人均碳排放量也存在波动上涨趋势.碳排放总量热点区域集中在成都和重庆,分别占总量约20%和25%,冷点区域为雅安市.碳排放总量和地均碳排放均存在显著的空间差异,人均碳排放的莫兰指数为正,呈现明显的空间聚集格局.整体上,人均碳排放表现出东北低-西南高的空间结构特征,南充,遂宁,广安是低低聚集区域.城市群中各个城市的影响因素显示出时空异质性,能源强度、经济发展水平、人口规模对城市的碳排放都有明显正向作用,在成渝中西部城市作用强度大;而城市化水平的正向影响较弱,对成渝东部城市影响较强.     

基于InVEST-PLUS模型的碳储量空间关联性及预测——以广东省为例

构建土地利用碳储量数据库,基于InVEST模型Carbon模块,得到广东省1990~2020年碳储量时空分布情况.用Moran’s I指数和Getis-Ord Gi^*分析格网尺度下碳储量时空分布特征,用Anselin Local Moran’s I得到LISA集聚图.然后运用PLUS模型和14个土地利用驱动因子预测2050年土地利用及其碳储量分布.结果表明,土地利用变化直接影响区域碳储量高低,林地、草地等具有生态服务功能地类碳密度最高,分别是188.44,329.34Mg/hm².碳储量空间格局整体呈现出中部低、北部高、东西中等的特点.碳储量空间分布特征与土地利用特征一致,碳储量显著高值集聚区域分布在建设用地少、生态用地多且连片的粤北地区,显著低值区域分布在国土开发强度和生态用地破碎化程度高的珠三角地带.在自然发展情景下,到2050年广东省土地利用碳储量将减少4327.21万Mg,随着国土空间进一步开发,环珠江口沿岸城市碳储量持续下降.增加植被生态系统碳储量,是实现碳中和的重要手段之一.要继续维持粤北山区生态保护屏障的重要地位,减缓珠三角城市土地开发强度,提高建设用地集约节约能力,形成平衡协调的土地利用和碳储量格局.     

铁盐浸渍强化污泥活性炭-甲醇热质传递特性

针对以市政污泥为核心的炭素前驱体开展原位铁盐浸渍磁修饰,通过响应曲面试验设计优化并制备了新型原位浸渍炭IM-WNC;以成品炭的后浸渍磁修饰炭PM-WNC为参比,考察了原位浸渍与后浸渍磁修饰过程对污泥活性炭-甲醇工质对的吸附/解吸速率、吸附等温线、吸附床传热性能、制冷量及制冷功率等方面的影响。结果表明:与后浸渍过程相比,原位铁盐浸渍有利于保持污泥炭总孔容积(0.6608cm³/g)及比表面积(1122m²/g)水平,能显著提升致密化污泥炭IM-WNC的导热系数(600kg/m³,4.586W/(m·K))、甲醇Sokoda&Suzuki平衡吸附量((528.74±15.86)mg/g)和Langmuir最大吸附量((673.99±13.52)mg/g)。升温脱附与冷却吸附循环体系内,IM-WNC致密化吸附床中心温度峰谷差值可达到69.07℃。当循环时间为76min,解吸温度为100℃时,IM-WNC吸附制冷床的制冷量和制冷功率分别达到501.43kJ/kg和799.06kJ/(kg·h),较PM-WNC分别提升了15.61%和18.69%。     

Ambient volatile organic compounds at a receptor site in the Pearl River Delta region: Variations, source apportionment and effects on ozone formation

We present the continuously measurements of volatile organic compounds（VOCs） at a receptor site（Wan Qing Sha, WQS） in the Pearl River Delta（PRD） region from September to November of 2017. The average mixing ratios of total VOCs（TVOCs） was 36.3 ± 27.9 ppbv with the dominant contribution from alkanes（55.5%）, followed by aromatics（33.3%）. The diurnal variation of TVOCs showed a strong photochemical consumption during daytime,resulting in the formation of ozone（O₃）. Five VOC sources were ...     

Impact of pre-oxidation on the formation of byproducts in algae-laden water disinfection: Insights from fluorescent and molecular weight

Pre-oxidation has been reported to be an effective way to remove algal cells in water, but the released algal organic matter (AOM) could be oxidized and lead to the increment in disinfection by-product (DBP) formation. The relationship between pre-oxidation and AOM-derived DBP formation needs to be approached more precisely. This study compared the impact of four pre-oxidants, ozone (O₃), chlorine dioxide (ClO₂), potassium permanganate (KMnO₄) and sodium hypochlorite (NaClO), on the formation of nitrogenous (N-) and carbonaceous (C-) DBPs in AOM chlorination. The characterization (fluorescent properties, molecular weight distribution and amino acids concentration) on AOM samples showed that the characterization properties variations after pre-oxidation were highly dependent on the oxidizing ability of oxidants. The disinfection experiments showed that O₃ increased DBP formation most significantly, which was consistent with the result of characterization properties variations. Then canonical correspondent analysis (CCA) and Pearson's correlation analysis were conducted based on the characterization data and DBP formation. CCA indicated that C-DBPs formation was highly dependent on fluorescent data. The formation of haloacetic acids (HAAs) had a positive correlation with aromatic protein-like component while trichloromethane (TCM) had a positive correlation with fulvic acid-like component. Pearson's correlation analysis showed that low molecular weight fractions were favorable to form N-DBPs. Therefore, characterization data could provide the advantages in the control of DBP formation, which further revealed that KMnO₄ and ClO₂ were better options for removing algal cells as well as limiting DBP formation.     

Interactions between lead(II) ions and dissolved organic matter derived from organic fertilizers incubated in the field

This work was to study composition characteristics and the subsequent effect on the lead (Pb) binding properties of dissolved organic matter (DOM) derived from seaweed-based (SWOF) and chicken manure organic fertilizers (CMOF) during a one-year field incubation experiment using the excitation-emission matrix-parallel factor (EEM-PARAFAC) and two-dimensional correlation spectroscopy (2DCOS) analysis. Results showed that high aromatic and hydrophobic fluorescent substances were enriched in CMOF-derived DOM and SWOF-derived DOM and enhanced over time. And phenolic groups in the fulvic-like substances for SWOF-derived DOM and carboxyl groups in the humic-like substances for CMOF-derived DOM had the fastest responses over time, respectively. Moreover, both non-fluorescent polysaccharides and fluorescent humic-like substances or fulvic-like substances with aromatic (C=C) groups first participated in the binding process of Pb to SWOF-derived DOM on day 0 and 180 during the lead binding process. In contrast, humic-like substances associated with aromatic (C=C) and phenolic groups gave a faster response to Pb binding on day 360. Regarding CMOF-derived DOM, the fulvic-like substances associated with aromatic (C=C) and carboxylic groups displayed a faster response to Pb ions on day 0. Nonetheless, polysaccharides and humic-like associated with phenolic groups had a faster response on days 180 and 360. It is noteworthy that the polysaccharides, which participated in Pb binding to CMOF-derived DOM, posed a higher risk of Pb in the environment after 360 days. Therefore, these findings gave new insights into the long-term applications of commercial organic fertilizers for the amendment of soil.     

Roles of semivolatile and intermediate-volatility organic compounds in secondary organic aerosol formation and its implication: A review

Secondary organic aerosol (SOA) is a very important component of fine particulate matter (PM_2.5) in the atmosphere. However, the simulations of SOA, which could help to elucidate the detailed mechanism of SOA formation and quantify the roles of various precursors, remains unsatisfactory, as SOA levels are frequently underestimated. It has been found that the performance of SOA formation models can be significantly improved by incorporating the emission and evolution of semivolatile and intermediate-volatility organic compounds (S/IVOCs). In order to explore the roles of S/IVOCs in SOA formation, this study reviews some simulation models which could consider S/IVOCs for SOA formation as well as the development of emission inventories of S/IVOCs and S/IVOC modules for SOA formation. In addition, the future research directions for simulations of the effect of S/IVOCs on SOA formation are suggested.