Effect of NOx and SO2 on the photooxidation of methylglyoxal: Implications in secondary aerosol formation

Methylglyoxal(CH_3COCHO,MG),which is one of the most abundant α-dicarbonyl compounds in the atmosphere,has been reported as a major source of secondary organic aerosol(SOA).In this work,the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at(293±3) K,atmospheric pressure,(18±2)% relative humidity,and under different NOx and SO_2.Particle size distribution was measured by using a scanning mobility particle sizer(SMPS) and the results showed that the addition of SO_2 can promote SOA formation,while different NOx concentrations have different influences on SOA production.High NOx suppressed the SOA formation,whereas the particle mass concentration,particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO_2.In addition,the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO_2 and MG/OH/NOx/SO_2 reaction systems were detected by gas chromatography mass spectrometry(GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy(ATR-FTIR) analysis.Two products,glyoxylic acid and oxalic acid,were detected by GC-MS.The mechanism of the reaction of MG and OH radicals that follows two main pathways,H atom abstraction and hydration,is proposed.Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra.Incorporation of NOx and SO_2 influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment.     

我国SO_2和NO_X排放强度地理分布和历史趋势

根据我国燃料消费、燃料的含硫量和硫与氮氧化物排放因子，计算我国各地区ＳＯ_２和ＮＯ_Ｘ排放强度地理分布。结果指出，我国原煤含硫量为１．１２％。１９９０年全国ＳＯ_２和ＮＯ_Ｘ的排放量分别为１７５１．８万ｔ和８４２．２万ｔ，排放强度最大的地区是中东部地区，即辽宁、河北、山东、山西和浙江。这些地区平均排放强度大于７ｔ／ｋｍ￣２·ａ。还估算了全国１９５０～１９９０年ＳＯ_２和ＮＯ_Ｘ历年的排放量。     

酸沉降破坏材料造成的经济损失的估算研究

酸沉降对材料的破坏和其经济损失估算是国际上酸沉降研究领域听一个重要课题，国内在经方面的研究较少，文章通过对“两广酸沉降破坏材料造成的经济损失的估算”研究，提出了了一套较实用的经济损失估算方法。     

铅酸蓄电池行业生产者责任延伸制在我国实施的难点和解决方案

为解决我国废弃产品环境污染问题和再生资源循环利用的困境,加快生态文明建设和循环经济发展,国务院现已推行生产者责任延伸制度。该项制度的推行实施,可减轻环境治理负担,推动循环经济和清洁生产模式,促进企业技术升级,但该项制度在具体实施过程中尚存在一些问题。以铅蓄电池行业为例,存在的主要问题包括相关制度不健全、回收利用体系不完善、缺乏多部门联动监管机制和有效的经济激励政策等。针对上述问题,结合河南省的废铅蓄电池收集处理制度试点工作,提出铅酸蓄电池行业生产者责任延伸制实施的建议方案,为生产者责任延伸制度更好地推行和实施提供参考。     

Variation of low molecular weight organic acids in precipitation and cloudwater at high elevation in South China

To investigate the sources and chemical behaviors of carboxylic acids in Southern China, precipitation and corresponding cloudwater samples were collected in an acid rain-prone area of Mount Heng. The carboxylic acid levels in the samples were measured, and the concentration patterns were evaluated with respect to temporal and seasonal variations. Formic and acetic acids were predominant among the carboxylic acids identified for both precipitation and cloudwater. Most of the organic acids in the precipitation had a clear seasonal pattern, reaching higher levels during the warm season; these higher levels were attributed to the stronger source strength of biogenic emissions during this season. The cloud–fog samples did not display a similar trend. A distinctive diurnal pattern in carboxylic acids was only observed in the precipitation samples during the warm season. In cloud–fog, the ratio of formic to acetic acid differed considerably with time, with these values varying little in the precipitation samples. This result indicates that the organic acids in precipitation originate consistently from primary sources throughout the entire period, while those in cloud are mainly associated with direct emissions in the earlier stage and with secondary sources in the later period.     

Origin and distribution of trace elements in high-elevation precipitation in southern China

Introduction

During a 2009 investigation of the transport and deposition of trace elements in southern China, 37 event-based precipitation samples were collected at an observatory on Mount Heng, China (1,269?m asl).

Methods

Concentrations of trace elements were analyzed using inductively coupled plasma?Cmass spectrometry and the wet deposition fluxes were established. A combination of techniques including enrichment factor analysis, principal component analysis, and back trajectory models were used to identify pollutant sources.

Results

Trace element concentrations at Mount Heng were among the highest with respect to measured values reported elsewhere. All elements were of non-marine origin. The elements Pb, As, Cu, Se, and Cd were anthropogenic, while Fe, Cr, V, Ba, Mn, and Ni were of mixed crustal/anthropogenic origin. The crustal and anthropogenic contributions of trace elements were 12.8 % (0.9?~?17.4 %) and 87.2 % (82.6?~?99.1 %), with the maximum crustal fraction being 17.4 % for Fe. Coal combustion, soil and road dust, metallurgical processes, and industrial activities contributed to the element composition.

Conclusions

Summit precipitation events were primarily distant in origin. Medium- to long-range transport of trace elements from the Yangtze River Delta and northern China played an important role in wet deposition at Mount Heng, while air masses from south or southeast of the station were generally low in trace element concentrations.     

有机化学品不同温度下(过冷)液体蒸气压预测模型的建立与评价

(过冷)液体蒸气压(PL)是评价化学品在环境中分配、迁移和归趋行为的重要参数。PL具有较强的温度依附性。发展一种能够精确预测不同环境温度下化学品PL的方法,有助于填补化学品生态风险评估的大量数据缺失。本研究收集整理了661种有机化合物在不同温度下(200~830 K)共计10 478个log PL值。在此基础上,采用偏最小二乘(PLS)回归和支持向量机(SVM)方法,构建了PL的线性和非线性预测模型。结果表明:2种模型均具有良好的拟合度、稳健性及预测能力,SVM模型的预测性能略高于PLS模型(PLS:R2adj.tra=0.912,RMSEtra=0.477,Q2ext=0.910;SVM:R2adj.tra=0.997,RMSEtra=0.092,Q2ext=0.967)。机理分析表明,温度是影响PL的主要因素,温度越高,蒸气压越大;其次,X1sol也影响PL大小,X1sol用来描述分子间的色散作用,分子间色散力越小,蒸气压越大;此外,化合物的氢键个数、极性和分子构型等因素也影响PL大小。采用Wiliams plot方法表征了PLS模型应用域。所建立的模型可用来预测烷烃、烯烃、醇、酮、羧酸、苯、酚、联苯、卤代芳香烃、含N化合物及含S化合物在不同温度下的PL数据。     

Particle number size distribution and new particle formation: New characteristics during the special pollution control period in Beijing

New particle formation is a key process in shaping the size distribution of aerosols in the atmosphere.We present here the measurement results of number and size distribution of aerosol particles (10-1...     

Effect of F,Cl, Br and I substitution on the BphB enzyme for the degradation of halogenated biphenyls,revealed by quantum and molecular mechanics

Halogenated biphenyls are worldwide persistent pollutants of great environmental concern. In particular, polychlorinated biphenyls and polybrominated biphenyls have been globally used for industrial purposes until they were found highly toxic, mutagenic and carcinogenic to humans. Therefore, ecological strategies to remove halogenated biphenyls, such as enzyme-catalyzed degradation, are needed. Here, we studied the effect of substitution of F, Cl, Br or I at the 4,4′-positions of 2,3-dihydro-2,3-dihydroxybiphenyl-2,3-dehydrogenase (BphB) on the degradation of halogenated biphenyls by quantum and molecular mechanics. Results show that Boltzmann-weighted average degradation barriers of substituted BphB are all lower than the unsubstituted biphenyl, except for chlorinated biphenyl. The roles of residues nearby the active site, e.g., isoleucine89, asparagine115, serine142, asparagine143, proline184, methionine187 and threonine189, were also investigated.