初论元素富集成矿的地球化学机理—以岩浆热液矿床的形成为例

元素富集成矿的过程实质上是元素在地球不同圈层和不同相以及不同集合体之间分配的结果。元素的富集起始于地球形成的初期。对于大多数金属成矿元素 ,地壳特别是上地壳是大多数矿石和矿胎的储库 ,地壳丰度是元素富集成矿的物质基础。元素在地质体系演化共存相间的分配是元素富集成矿的关键过程。对于以侵入体为中心的热液矿床的形成 ,岩浆部分熔融、结晶分异、液态分离、挥发分分离以及气液相不混溶等过程能够导致金属元素最终达到矿石级的富集。挥发分则是元素富集成矿的重要制约因素     

Isomer distribution of nitrotriphenylenes in airborne particles, diesel exhaust particles, and the products of gas-phase radical-initiated nitration of triphenylene

The formation of mutagenic nitro-polycyclic aromatic hydrocarbons (NPAHs) 1- and 2-nitrotriphenylene (1- and 2-NTP) via gas-phase OH or NO₃ radical-initiated reactions of triphenylene was demonstrated for the first time using a flow reaction system. In contrast with the results of conventional electrophilic nitration, 2-NTP was formed in larger yield than 1-NTP, but this is consistent with the mechanism proposed for gas-phase radical-initiated nitration of PAH. In diesel exhaust particle (DEP) samples, both 1- and 2-NTP were identified and their concentrations determined, as well as 1-nitropyrene (1-NP), which is a representative combustion-derived NPAH: the mean concentrations of 1-NTP, 2-NTP, and 1-NP were 4.7, 1.9, and 32 pmol mg_DEP^–1, respectively. The mean 2-NTP/1-NTP, 1-NTP/1-NP, and 2-NTP/1-NP ratios in samples of airborne particles collected in a residential area in Osaka, Japan, were>1.55,<0.25, and 0.37, respectively; these values are much higher than those of the DEP samples. This finding indicates that there is another source for airborne NTPs, especially 2-NTP, apart from diesel exhaust. These results strongly suggest that airborne NTPs originate from atmospheric processes such as radical-initiated reactions of triphenylene, and this has a significant influence on the atmospheric occurrence of NTPs.     

PM10冲击采样器切割头设计参数对切割粒径的影响

本文从颗粒在气流中的受力情况分析入手 ,得到冲击采样器中喷嘴喷出后颗粒的运动轨迹方程以及运动轨迹与采样器切割头设计参数的关系式。分析了PM10空气采样器的切割原理 ,并利用数值计算研究颗粒在不同的流量、喷嘴尺寸及喷嘴与冲击板的距离下的运动轨迹 ,从而得到切割头设计参数对切割粒径的影响     

Association of the mutagenicity of airborne particles with the direct emission from combustion processes investigated in Osaka, Japan

The association of the direct-acting mutagenicity of soluble organic fraction of airborne particles toward Salmonella typhimurium YG1024 strain with the direct emission was investigated at a roadside and at a residential area in Osaka, Japan. The direct-acting mutagenicity was evaluated as mutagenic activity per unit volume of ambient air (rev m⁻³) and/or that per airborne particulate weight collected on a filter (rev mg⁻¹). The annual or diurnal changes of the mutagenicity of airborne particles at the residential site showed similar patterns to those of some gaseous pollutants such as NO₂ and SO₂, which were emitted from combustion processes. This result indicates that the mutagenicity is mainly attributable to the primary emissions. From the analysis of the relationship between the wind sector and the mutagenic intensity, rev m⁻³ and rev mg⁻¹ values were strongly affected by the emissions from the fixed sources and from the mobile sources, respectively. The rev m⁻³ value and concentration of 1-nitropyrene (1-NP) in unit per m³ at the roadside were a factor of 2.6 and 2.8 higher than those at the residential site, respectively, but the rev mg⁻¹ value and concentration of 1-NP in unit per mg at the roadside were substantially comparable to those at the residential area. These observations suggest that the characteristics of the airborne particles can be attributed to the automotive emissions even at the suburban area.     

南京地区相对湿度对气溶胶含量的影响

为了研究南京地区相对湿度对气溶胶的影响,利用位于南京信息工程大学的拉曼-瑞利-米氏激光雷达,分析湿度廓线对消光系数的影响;利用2014年3月~2015年2月国控点环境监测数据对可吸入颗粒物浓度特征进行统计,并与相对湿度进行逐月和四季对比分析,并计算各参数之间的相关系数,以期为南京市的城市布局与规划、大气污染治理等提供更多参考.结果表明,低空气溶胶的消光系数廓线与相对湿度廓线变化趋势高度一致,地面相对湿度与可吸入颗粒物浓度在一定湿度范围（以不发生重力沉降为界限）内,相对湿度越大越有利于颗粒物的形成,超过这个范围,相对湿度越大,颗粒物浓度越低,在南京地区,对于PM₁₀来说,这个界限在40%~49%,对于PM_2.5来说,这个界限在50%~59%.     

基于气候响应关系研究火干扰对兴安落叶松直径结构的 影响

以大兴安岭地区兴安落叶松（Larix gmelinii）为研究对象,分别选取1987年、2003年和2015年火干扰区域及其附近未受火干扰区域设置典型样地,基于树轮数据和调查数据重建历史直径结构,构建兴安落叶松树木生长与气候因子的相关关系,探讨气候变化背景下火干扰对兴安落叶松直径结构的影响。研究结果表明：（1）火干扰下兴安落叶松直径结构呈正偏,高峰态分布。中度火干扰恢复15年后则呈现负偏、峰度值下降的趋势,而重度火干扰恢复15年后仍处于正偏高峰态分布,但随后趋向负偏,低峰态分布。（2）火干扰改变了兴安落叶松直径生长与气候之间的响应关系,中度火干扰下兴安落叶松生长与上年冬季温度呈显著负相关（p＜0.05）,随着火干扰强度增加,降水的抑制作用增强,重度火干扰下兴安落叶松直径生长与当年生长季（5—8月）、上年生长季（7—9月）和上年冬季（11—12月）降水呈显著负相关关系（p＜0.05）。不同恢复期内树木生长-气候因子关系也有所差异。中度火干扰下兴安落叶松与生长季温度的关系由火干扰初期正相关转变为中期（恢复15年）负相关（p＜0.05）,与上年生长季降水的关系则转变为正相关关系（p＜0.05）;重度火干扰下兴安落叶松直径生长与上年冬季温度由恢复初期的负相关转变为后期（恢复31年）的正相关（p＜0.05）,与当年生长季降水转变为负相关（p＜0.05）。在未来气候变暖和火干扰事件增加的趋势下,兴安落叶松直径结构趋向负偏、高峰态分布。     

成都西南城郊黑碳和PM2.5 浓度变化特征及其影响因子

四川盆地是我国灰霾和大气污染易发和频发区之一,目前关于本地区黑碳气溶胶（black carbon,BC）的相关研究较少。利用2017年11月—2018年12月成都西南城郊地区黑碳气溶胶以及PM_2.5观测资料,结合气象资料和其他污染物浓度资料,分析BC和PM_2.5浓度,BC浓度在PM_2.5浓度中所占比例（黑碳占比）的季节、月、日变化特征及其影响因子。结果表明：（1）BC逐小时浓度范围为0.18—40.51 μg?m^?3,平均值为(5.26±4.68) μg?m^?3,本底浓度为3.34 μg?m^?3。PM_2.5逐小时浓度范围为1.00—344.50 μg?m^?3,平均值为(60.02±46.91) μg?m^?3,本底浓度为33.38 μg?m^?3。日变化均呈“白天低,早晨、夜间高”的变化特征,其中冬季浓度最高,春、秋季次之,夏季浓度最低。（2）黑碳占比均值为9.16%±5.13%,白天黑碳占比低,夜间黑碳占比高,且夏季最高,冬季最低。随着空气污染加重,冬季占比缓慢增加,其他三季占比减小。（3）BC与NO₂和CO相关性较好,表明西南城郊BC排放主要受机动车尾气、生物质燃烧影响。BC和SO₂相关系数偏小,燃煤等工业源排放对西南城郊BC的贡献较小。（4）风速、温度和湿度与BC浓度均有很好的相关性,其中风速对BC浓度的影响最大,当风速小于2.0 m?s^?1时,BC浓度值明显偏高;BC浓度大于20.00 μg?m^?3的高值区主要集中在西北、西南以及东北风向上,即：偏东北方向市中心大气中的污染物,以及西南方向远郊地区的污染物可能对西南城郊高浓度黑碳的贡献更大。     

成都市PM2.5中无机组分与硝酸盐氮氧同位素变化特征

2013年1月12日～2013年1月23日和2014年8月10日～2014年8月21日在成都市城东成都理工大学校园内按昼夜采集PM_(2.5)样品,分析了PM_(2.5)样品的质量浓度、9种水溶性无机离子含量和硝酸盐的δ~(15)N和δ~(18)O。结果表明,采样期间成都市PM_(2.5)冬、夏季的质量浓度分别为161～677μg/m~3(360±118μg/m~3)和87～137μg/m~3(92±18μg/m~3),冬季超标2～9倍,属于重度污染,夏季超标1～2倍,属于轻度污染; SO_4~(2-)、NO_3~-和NH_4~+(SNA)的质量浓度占总水溶性无机离子和PM_(2.5)质量浓度的比值冬夏季分别为72%±14. 3%和65%±9. 2%,21. 1%±2. 5%和30. 3%±6. 9%,是主要的无机离子组分。结合离子相关性分析,SNA的存在形式在白天以(NH_4)_2SO_4或NH_4HSO_4为主,部分以NH_4NO_3的形式存在,而在夜间则以NH_4NO_3为主,部分以(NH_4)_2SO_4或NH_4HSO_4形式存在。成都市PM_(2.5)中硝酸盐的δ~(15)N和δ~(18)O呈冬季高、夏季低的特征。冬季,硝酸盐来源于燃煤和机动车尾气;夏季,硝酸盐来源于机动车尾气、燃煤和农业土壤释放,根据其[NO_3~-]/[SO_4~(2-)]值说明成都市冬夏季均以固定污染源(燃煤)为主,移动污染源(机动车尾气)为辅。成都市冬季大气颗粒物中硝酸盐主要由NO_x经O_3氧化形成,夏季主要经·OH氧化形成硝酸盐或N_2O_5水解生成硝酸盐。     

Characterization of submicron particles during autumn in Beijing, China

In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles(NR-PM_1) in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer(HR-ToF-AMS). The results showed the average NR-PM_1 mass concentration to be 56.4 ± 58.0 μg/m~3, with a peak at 307.4 μg/m~3. Due to the high frequency of biomass burning in autumn, submicron particles significantly increased in organic content, which accounted for 51% of NR-PM_1 on average. Secondary inorganic aerosols(sulfate + nitrate + ammonium) accounted for 46% of NR-PM_1, of which sulfate,nitrate, and ammonium contributed 15%, 20%, and 11%, respectively. To determine the intrinsic relationships between the organic and inorganic species, we used the positive matrix factorization(PMF) model to merge the high-resolution mass spectra of the organic species and NO+and NO_2~+ions. The PMF analysis separated the mixed organic and nitrate(NO+and NO_2~+) spectra into four organic factors, including hydrocarbon-like organic aerosol(HOA), oxygenated organic aerosol(OOA), cooking organic aerosol(COA), and biomass burning organic aerosol(BBOA), as well as one nitrate inorganic aerosol(NIA) factor. COA(33%) and OOA(30%) contributed the most to the total organic aerosol(OA) mass, followed by BBOA(20%) and HOA(17%). We successfully quantified the mass concentrations of the organic and inorganic nitrates by the NO+and NO2+ions signal in the organic and NIA factors. The organic nitrate mass varied from 0.01-6.8 μg/m~3, with an average of 1.0 ±1.1 μg/m~3, and organic nitrate components accounted for 10% of the total nitrate mass in this observation.     

Soot reduction by addition of dimethyl carbonate in normal and inverse ethylene diffusion flames: Nanostructural evidence

Oxygenated fuel represents an attractive alternative as an additive for reducing soot emissions.Dimethyl carbonate(DMC) is an oxygenated compound which is a good option to reduce soot,but the detailed characteristics of soot produced from combustion of hydrocarbon fuels blended with DMC are still lacking. The present research studied the nanostructure and reactivity of soot particles in ethylene/DMC normal and inverse diffusion flames. High resolution transmission electron microscopy(HRTEM), X-ray diffraction(XRD), and thermogravimetric analysis(TGA)were used to analyze the nanostructure and reactivity of soot. It was found that DMC addition was effective in decreasing the average weights of soot formed in flames. The results of HRTEM images showed that soot particles obtained with DMC addition showed liquid-like material and tight bonding, and exhibited more highly disorganized layers, which give it higher reactivity than soot obtained without DMC addition. Furthermore, HRTEM was used to analyze soot fringe characteristics consisting of fringe tortuosity, fringe length, and fringe separation. XRD was used to crosscheck the results for fringe separation, and was consistent with HRTEM results. In addition, the mass loss curve of TGA experiments showed that DMC addition could enhance the reactivity of soot particles.