天地一体化遥感监测大气污染技术进展

天地一体化遥感监测技术通过地基和卫星融合互补,成为研究大气污染来源、传输和影响的重要方法.但目前国外主导的地基和卫星遥感算法不适应国内复杂大气环境,其数据可靠性尚需验证.为进一步推动国内大气研究自主性,厘清天地一体化遥感监测技术发展现状,对相应的平台建设、算法研发及应用实例进行介绍.结果表明:①可通过地基观测网络实时连续监测大气污染物的浓度（柱总量）/廓线信息,目前国内组建并运行了CNEMC空气质量监测网络和USTC地基遥感网络.②可通过紫外-可见波段卫星载荷获取全球/区域尺度大气污染物的浓度（柱总量）/廓线产品,GF-5搭载的EMI填补了国内该类载荷的空白,基于DOAS（BOAS）的柱总量反演算法、基于OE的垂直廓线反演算法是当下国际主流业务算法.③天地一体化遥感监测技术以高精度、广覆盖、准定位的优势得到快速发展,可为亟需解决的大气污染治理成效评估、作用机理研究、区域传输测算及精准溯源等难题提供技术支持.研究显示,天地一体化遥感监测技术需以应用化和业务化为导向,加快观测平台硬件建设,加强相关反演算法研发,深入融合多平台数据,全面推进大气遥感监测技术的立体化和系统化发展.      

非二氧化碳温室气体氧化亚氮的卫星遥感研究综述

氧化亚氮(N₂O)已成为全球第三大温室气体,氮氧化物污染与治理也成为我国“十四五”生态环保工作重点,气候变化评估与环境保护均对N₂O卫星遥感提出了较高的要求.本文回顾了N₂O卫星遥感的主要进展,卫星载荷方面,从天底、临边、掩星3种观测方式介绍了N₂O卫星观测的历史进程;反演算法方面,根据观测方式的不同分别介绍了最优估计算法、剥洋葱算法、差分光学吸收光谱法.相较于国际上N₂O卫星遥感起步早且已具备了较为成熟的理论和技术,我国的N₂O卫星遥感监测能力还有较大的发展空间.本文通过对研究现状的梳理和总结,提出了N₂O卫星遥感的发展趋势和建议,并对未来发展前景进行了展望.     

基于机器学习的二氧化碳卫星反演方法

基于机器学习模型在分析数据并学习预测方面的优势,提出了一种基于机器学习的短波红外通道CO₂卫星遥感反演方法,以卫星观测辐亮度、气溶胶光学厚度、温度构建训练数据集,采用前馈神经网络与量化共轭梯度算法进行训练学习,构建了短波红外通道卫星CO₂反演模型,并利用GOSAT卫星观测光谱数据反演了CO₂浓度.反演结果与TCCON站点观测数据进行了比对,结果表明:卫星与地面观测的相关性优于0.86,平均误差小于2.5×10^-6,验证了反演方法的有效性.     

MODIS卫星遥感AOD反演近地面“湿”消光系数新模型的构建及应用

针对气溶胶含量随高度呈负指数递减这一假设存在的问题,通过对Mie散射激光雷达探测资料的系统分析和总结,论证了Logistic曲线能更好地表征大气消光系数在边界层内的垂直演变特征.在对MODIS卫星遥感气溶胶光学厚度(AOD)系统偏差进行校正的基础上,将大气消光系数的模拟值与实测值之间离差平方和最小作为目标函数,利用小波协方差法计算混合层高度,以订正后的AOD和混合层高度作为约束条件,再用免疫进化算法优化目标函数中的参数,据此提出了MODIS卫星遥感AOD反演近地面"湿"消光系数的新模型.基于成都市2013年6月—2014年5月的MODIS卫星遥感AOD资料及同时次的Mie散射激光雷达探测数据和地面细颗粒物浓度资料的实例分析表明,新模型反演得到的近地面大气"湿"消光系数与近地面细颗粒物质量浓度之间的相关系数在四季均能稳定在0.6以上.     

基于MODIS数据反演江浙皖地区气溶胶光学厚度

气溶胶是气候变化和大气污染的重要影响因素。人们发现卫星遥感为大面积获取气溶胶光学厚度提供了手段,同时卫星遥感的气溶胶光学厚度弥补了地面观测空间覆盖不足的缺陷。文章首先介绍了使用暗像元法反演气溶胶光学厚度的算法和计算流程,利用传统的暗像元法和改进的暗像元法(即V5.2算法)反演江浙皖地区(29～33°N;116～120°E)气溶胶光学厚度的空间分布,并对两种算法所得结果进行比较与分析。结果表明:暗像元法基本可以反映出该区域气溶胶光学厚度的空间分布特点,尤其是在浓密植被区卫星反演得到的结果与(AERONET)太阳光度计的观测值基本相近。但是在城市地区,该算法得到的结果与观测值存在一定的偏差,有待于进一步改善。     

微波超视距雷达大气波导环境

针对岸基/舰载微波超视距雷达远距离海上低空或海面目标探测的实际需求,首先对大气波导的直接测量和遥感反演等探测方法进行了分析比较,基于对大气波导形成机制和中尺度数值预报模式的分析,指出了有效预报大气波导需要解决的3个基本问题,最后对微波超视距雷达电波传播模型和评估方法进行了讨论。     

基于GF-4卫星的长三角城市群PM2.5遥感反演

基于静止卫星高分四号（GF-4）遥感数据,利用6SV辐射传输模型与暗目标算法进行高空间分辨率气溶胶光学厚度（AOD）遥感反演;在此基础上,结合地面监测站大气细颗粒物（PM_2.5）浓度、气象资料等数据,采用物理订正方法及线性混合效应模型,实现长三角城市群区域大尺度空间连续的PM_2.5浓度遥感反演;最后利用十折交叉验证法对反演精度进行验证.结果表明：GF-4反演的AOD结果分辨率较高,空间连续性好,与AERONET地基监测相关性R达到0.82;利用GF-4 AOD的PM_2.5估算模型精度较高,模型估算PM_2.5浓度与地面实测数据拟合度R²为0.74;在分春夏秋冬4个季节建模情景下,交叉验证R²依次为0.67,0.59,0.63和0.72,平均绝对误差MAE为10.40,7.42,10.10,13.34μg/m³,表明GF-4卫星适用于区域PM_2.5浓度监测.     

大气气溶胶主被动遥感探测应用技术进展

大气气溶胶广泛影响着地球的气候与环境,尤其是日益严重的颗粒物污染已对公众健康和生态安全构成了巨大的威胁。面对我国空气重污染的现状,大气污染治理急需对气溶胶及其光学特性进行大范围、高频次、高精度、立体的遥感监测和定量分析。目前,气溶胶遥感监测有多波段、多角度、偏振等被动探测方法,也有激光雷达结合高光谱、偏振的主动探测方法。本文在分析国内外大气激光雷达卫星载荷的基础上,分析了目前基于主动、被动遥感探测手段的气溶胶遥感监测应用研究进展,研究发现激光主动探测在大气环境定量监测中的作用更加突出,主被动结合、多手段综合是大气环境监测卫星的发展方向。     

基于FY-4A卫星数据反演气溶胶光学厚度及分析应用

风云四号A星（FY-4A）是我国新一代静止气象卫星,多通道扫描成像辐射计（AGRI）是风云四号静止气象卫星的主要载荷之一.为探究FY4A数据用于气溶胶光学厚度（AOD）反演的可行性,基于FY-4A/AGRI数据,利用暗像元算法对2019年2月23~26日及10月27~30日京津冀地区AOD进行反演研究,并与AERONET地基观测AOD数据进行了对比分析.结果表明,基于FY-4A数据及构建响应函数库,通过暗像元方法能较好的反演出京津冀地区气溶胶空间分布;AOD主要的高值区体现在京津冀中南部地区并向周边郊区逐渐降低,在AOD值较大时此特征较为明显;将反演值与同期AERONET地基观测数据对比验证,相关系数达到0.869,均方根误差为0.221,表明AOD反演值与观测值吻合较好,FY-4A卫星数据反演AOD具有一定可行性.     

基于FY-4A卫星数据反演气溶胶光学厚度及分析应用

风云四号A星（FY-4A）是我国新一代静止气象卫星,多通道扫描成像辐射计（AGRI）是风云四号静止气象卫星的主要载荷之一.为探究FY4A数据用于气溶胶光学厚度（AOD）反演的可行性,基于FY-4A/AGRI数据,利用暗像元算法对2019年2月23~26日及10月27~30日京津冀地区AOD进行反演研究,并与AERONET地基观测AOD数据进行了对比分析.结果表明,基于FY-4A数据及构建响应函数库,通过暗像元方法能较好的反演出京津冀地区气溶胶空间分布;AOD主要的高值区体现在京津冀中南部地区并向周边郊区逐渐降低,在AOD值较大时此特征较为明显;将反演值与同期AERONET地基观测数据对比验证,相关系数达到0.869,均方根误差为0.221,表明AOD反演值与观测值吻合较好,FY-4A卫星数据反演AOD具有一定可行性.     

Vertical distribution and temporal evolution of formaldehyde and glyoxal derived from MAX-DOAS observations: The indicative role of VOC sources

Formaldehyde (HCHO) and glyoxal (CHOCHO) are important oxidization intermediates of most volatile organic compounds (VOCs), but their vertical evolution in urban areas is not well understood. Vertical profiles of HCHO, CHOCHO, and nitrogen dioxide (NO₂) were retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations in Hefei, China. HCHO and CHOCHO vertical profiles prefer to occur at higher altitudes compared to NO₂, which might be caused by the photochemistry-oxidation of longer-lived VOCs at higher altitudes. Monthly means of HCHO concentrations were higher in summer, while enhanced amounts of NO₂ were mainly observed in winter. CHOCHO exhibited a hump-like seasonal variation, with higher monthly-averaged values not only occurred in warm months (July-August) but also in cold months (November-December). Peak values mainly occurred during noon for HCHO but emerged in the morning for CHOCHO and NO₂, suggesting that HCHO is stronger link to photochemistry than CHOCHO. We further use the glyoxal to formaldehyde ratio (GFR) to investigate the VOC sources at different altitudes. The lowest GFR value is almost found in the altitude from 0.2 to 0.4 km, and then rises rapidly as the altitude increases. The GFR results indicate that the largest contributor of the precursor VOC is biogenic VOCs at lower altitudes, while at higher altitudes is anthropogenic VOCs. Our findings provide a lot more insight into VOC sources at vertical direction, but more verification is recommended to be done in the future.     

A tunable diode laser absorption spectrometer for formaldehyde atmospheric measurements validated by simulation chamber instrumentation

A tunable diode laser absorption spectrometer (TDLAS) for formaldehyde atmospheric measurements has been set up and validated through comparison experiments with a Fourier transform infrared spectrometer (FT-IR) in a simulation chamber. Formaldehyde was generated in situ in the chamber from reaction of ethene with ozone. Three HCHO ro-vibrational line intensities (at 2909.71, 2912.09 and 2914.46 cm^-1) possibly used by TDLAS were calibrated by FT-IR spectra simultaneously recorded in the 1600-3200 cm^-1 domain during ethene ozonolysis, enabling the on-line deduction of the varying concentration for HCHO in formation. The experimental line intensities values inferred confirmed the calculated ones from the updated HITRAN database. In addition, the feasibility of stratospheric in situ HCHO measurements using the 2912.09 cm^-1 line was demonstrated. The TDLAS performances were also assessed, leading to a 2σ detection limit of 88 ppt in volume mixing ratio with a response time of 60 sec at 30 Torr and 294 K for 112 m optical path. As part of this work, the room-temperature rate constant of this reaction and the HCHO formation yield were found to be in excellent agreement with the compiled literature data.     

基于OMI数据的中国中东部臭氧及前体物的时空分布

基于OMI卫星资料,分析了2005—2014年中国中东部地区对流层低层ρ(O₃)、对流层NO₂柱浓度及甲醛总柱浓度的时空演变趋势及相互关系. 结果表明:近10年来,中国中东部地区对流层低层ρ(O₃)呈上升趋势,2005年及2014年分别为60.64、69.43 μg/m3,年均增长率为1.6%;对流层低层ρ(O₃)增长的区域面积不断扩大,部分地区增长超23 μg/m3;呈春夏季高,冬季最低的分布趋势. 2005—2012年,对流层NO₂柱浓度呈上升趋势,2005年及2012年分别为4.41×1015、5.90×1015 mol/cm2,年均增长率为4.8%;2012年后呈下降趋势,下降的区域面积逐步扩大,部分地区降低约 15×1014 mol/cm2;呈冬季最高、夏季最低的分布特征;2005—2010年甲醛总柱浓度呈上升趋势,2005年及2010年分别为9.74×1015、1.59×1016 mol/cm2,年均增长率为12.6%,2010年后呈下降趋势;呈夏季最高、冬季最低的分布特征;甲醛总柱浓度增长的区域面积逐渐扩大. 利用甲醛与NO₂柱浓度比值探讨臭氧控制区的空间分布特征,表明鲁豫晋、京津冀、长三角及珠三角地区中心城市属于VOCs控制区,周围城市属于VOCs-NO_x协同控制区,其他地区属于NO_x控制区.      

Elimination of formaldehyde over Cu-Al2O3 catalyst at room temperature

Catalytic elimination of formaldehyde (HCHO) was investigated over Cu-Al2O3 catalyst at room temperature. The results indicated that no oxidation of HCHO into CO2 occurs at room temperature, but the adsorption of HCHO occurs on the catalyst surface.With the increase of gas hourly space velocity(GHSV) and inlet HCHO concentration, the time to reach saturation was shortened proportionally. The results of the in situ DRIFTS, Density functional theory calculations and temperature programmed desorption(TPD) showed that HCHO was completely oxidized into HCOOH over Cu-Al2O3 at room temperature. With increasing the temperature in a flow of helium, HCOOH was completely decomposed into CO2 over the catalyst surface, and the deactivated Cu-Al2O3 is regenerated at the same time. In addition, although Cu had no obvious influence on the adsorption of HCHO on Al2O3, Cu dramatically lowered the decomposition temperature of HCOOH into CO2. It was shown that Cu-Al2O3 catalyst had a good ability for the removal of HCHO, and appeared to be promising for its application in destroying HCHO at room temperature.     

基于DOAS地空观测的典型热带地区臭氧敏感性研究

为实现中国节能减排与产业经济协调发展的目标，本研究选取中国碳排放重要来源之一的能源密集型产业，采用空间全局自相关，标准差椭圆，空间局部自相关以及空间杜宾模型等方法对2007—2016年中国30个省域能源密集型产业格局、碳排放强度时空演变特征进行了分析，在空间溢出视角下对能源密集型产业结构演变的碳排放效应进行了探讨.结果表明：①空间自相关Moran''s I检验表明碳排放强度与能源密集型产业集聚均存在显著的空间正相关.②标准差椭圆表明，能源密集型产业有重心迁移的现象，但迁移效果不明显.③空间杜宾结果显示，能源密集型产业集聚与碳排放强度呈现"N"型曲线关系，能源密集型产业的集聚对碳排放强度的影响存在明显的空间溢出效应，人口数量和外商投资会显著抑制碳排放强度.     

Long-term observations of tropospheric NO2, SO2 and HCHO by MAX-DOAS in Yangtze River Delta area, China

Yangtze River Delta(YRD) area is one of the important economic zones in China. However,this area faces increasing environmental problems. In this study, we use ground-based multi-axis differential optical absorption spectroscopy(MAX-DOAS) network in Eastern China to retrieve variations of NO_2, SO_2, and formaldehyde(HCHO) in the YRD area. Three cities of YRD(Hefei, Nanjing, and Shanghai) were selected for long-term observations. This paper presents technical performance and characteristics of instruments, their distribution in YRD, and results of vertical column densities(VCDs) and profiles of NO_2, SO_2, and HCHO.Average diurnal variations of tropospheric NO_2 and SO_2 in different seasons over the three stations yielded minimum values at noon or in the early afternoon, whereas tropospheric HCHO reached the maximum during midday hours. Slight reduction of the pollutants in weekends occurred in all the three sites. In general trace gas concentrations gradually reduced from Shanghai to Hefei. Tropospheric VCDs of NO_2, SO_2, and HCHO were compared with those from Ozone Monitoring Instrument(OMI) satellite observations, resulting in R~2 of 0.606, 0.5432, and 0.5566, respectively. According to analysis of regional transports of pollutants, pollution process happened in YRD under the north wind with the pollution dissipating in the southeast wind. The feature is significant in exploring transport of tropospheric trace gas pollution in YRD, and provides basis for satellite and model validation.     

沿海城市秋季大气甲醛污染来源及其环境影响

基于大气综合观测站的气态污染物(HCHO、O₃、PAN、CO、NOx、异戊二烯)及气象要素(温度、湿度、风速、风向)等在线观测数据,研究沿海城市厦门秋季大气HCHO的时间变化特征及其关键影响因子,利用多元线性回归分析方法定量识别HCHO的主要来源,并估算HCHO对·OH生成的贡献.结果表明:HCHO平均浓度为(3.15±1.40)×10^-9,范围为(0.55～7.96)×10^-9,呈现明显“单峰”日变化特征,峰值出现在13:00左右.HCHO与O₃、PAN显著正相关;温度、湿度和UV是影响HCHO浓度的主要气象因素,强辐射、高温、低湿、低风速和西南风的条件促进了厦门大气HCHO的二次生成. HCHO小时光解量(PHCHO)范围为(0.01～3.02)×10^-9/h,平均PHCHO为0.61×10^-9/h,同时,大气HCHO光解成稳定分子H2和CO的速率是光解成自由基H·和HCO·速率的1.1～1.6倍.观测期间大气HCHO来源主要包括二次生成(39.2%)...     

华北农村夏季大气甲醛浓度变化特征

为研究华北农村大气污染状况,于2013年夏季和2014年夏季先后在华北两个农村站点——固城站、饶阳站,采用基于汉栖(Hantzsch)反应的在线甲醛荧光分析仪开展大气甲醛在线观测,结合同期φ(O₃)、φ(PAN)(PAN为过氧乙酰硝酸酯)、φ(CO)和光解速率系数等数据,分析φ(甲醛)日变化及其光解速率等特征. 结果表明:华北农村夏季大气甲醛污染较重. 固城站和饶阳站φ(甲醛)分钟均值范围分别为0.05×10-9 ~59.18 ×10-9和1.66×10-9 ~ 46.83×10-9,平均值分别为12.82×10-9±7.59×10-9和13.73×10-9±5.82×10-9,高于文献报道的国内外其他地区的观测值,与同期观测的φ(NO_x)相当. 两个站点φ(甲醛)具有典型的日变化特征,φ(甲醛)小时均值峰值(固城站为17.43×10-9,饶阳站为17.57×10-9)均出现在上午10:00左右,与φ(O₃)和φ(PAN)的日变化趋势相似,但峰值早1 h出现. 光解速率系数观测结果表明,两个站点甲醛光解过程主要发生在06:00—18:00,固城站甲醛小时光解量峰值(2.59×10-9)出现在11:00,饶阳站甲醛小时光解量于正午12:00达到峰值(3.00×10-9),甲醛光解成稳定分子的速率是光解成自由基速率的1.2~1.7倍. 研究表明,两个站点φ(甲醛)的变化主要受局地过程的影响,光化学生成是甲醛的重要来源.      

Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006-2011

Based on the observation by a Regional Air Quality Monitoring Network including 16 monitoring stations, temporal and spatial variations of ozone(O3), NO2and total oxidant(Ox) were analyzed by both linear regression and cluster analysis. A fast increase of regional O3concentrations of 0.86 ppbV/yr was found for the annual averaged values from 2006 to 2011 in Guangdong, China. Such fast O3increase is accompanied by a correspondingly fast NOx reduction as indicated by a fast NO2 reduction rate of 0.61 ppbV/yr. Based on a cluster analysis, the monitoring stations were classified into two major categories – rural stations(non-urban) and suburban/urban stations. The O3concentrations at rural stations were relatively conserved while those at suburban/urban stations showed a fast increase rate of 2.0 ppbV/yr accompanied by a NO2 reduction rate of 1.2 ppbV/yr. Moreover, a rapid increase of the averaged O3 concentrations in springtime(13%/yr referred to 2006 level) was observed, which may result from the increase of solar duration, reduction of precipitation in Guangdong and transport from Eastern Central China. Application of smog production algorithm showed that the photochemical O3production is mainly volatile organic compounds(VOC)-controlled. However, the photochemical O3production is sensitive to both NOx and VOC for O3pollution episode. Accordingly, it is expected that a combined NOx and VOC reduction will be helpful for the reduction of the O3 pollution episodes in Pearl River Delta while stringent VOC emission control is in general required for the regional O3 pollution control.