氧化亚氮与氮氧化物时空足迹模型研究

发布时间：2018-07-06 12:26

本文选题：农业施肥 + 化石燃料燃烧　；参考：《浙江大学》2016年博士论文

【摘要】：人类活动对自然氮循环过程的扰动导致活性氮大气排放急剧增长,明确其排放时空格局对气候变化减缓以及相应大气污染控制措施的制定具有重要意义。农业生产与化石燃料燃烧在全球人为大气活性氮排放中占比分别为56.5%、35.3%；我国来自农业施肥的温室气体氧化亚氮(N20)和来自化石燃料燃烧的二次细颗粒物主要前体物氮氧化物(NOx)是活性氮排放中的典型污染物。然而,由于空间数据的缺乏,N20和NOx排放源强的空间分布评估仍颇具挑战。生物地球化学过程模型、遥感技术的发展为活性氮空间评估提供了空间信息,但如何挖掘空间信息数据,进而量化活性氮排放时空规律,目前尚不明确。本文旨在从活性氮在不同时间与地域的生物地球化学与人类活动足迹视角,利用多源数据与统计建模手段破解数据缺乏难题,解析农业施肥N20与化石燃料燃烧NOx排放时空格局。在排放清单、生物地球化学模型与遥感反演方法综述基础上,以中国省市区域为空间尺度、最大数据可获取年份为时间边界,通过统计年鉴、研究论文等文献数据与全球遥感数据共享平台数据采集,研究了农业施肥的N20排放与化石燃料燃烧的NOx排放时空足迹评估模型。以我国典型特色经济作物毛竹为例,利用生物地球化学过程模型DeComposition-DeNitrification (DNDC)蒙特卡洛模拟数据样本,通过偏相关分析法筛选评估参数,进而采用逐步多元回归分析法构建了施肥N20排放计算模型,评估我国省域尺度毛竹林N20排放源强分布；通过DMSP/OLS夜间稳定灯光遥感数据与NOx排放相关性分析验证,开展了基于聚类分析的地域分区,构建了不同区域基于夜间灯光的燃烧源NOx排放回归模型,并采用基于空间自相关分析的Moran's1指数解析了NOx排放的空间集聚特征；通过农业施肥情景分析与区域问贸易流通隐含氮足迹的多区域投入产出分析探讨了N20与NOx足迹的管理对策。主要研究结论如下：(1)毛竹林施肥活性氮N20排放(E)时空格局与氮肥施用量(N)和降水量(P)显著相关。比选三种基于当前施肥N20排放影响理论的线性与非线性模型,最优排放评估模型为E=0.057 N-2.61×10-3P,在 96≤N≤298 kgN hm-2、700≤P≤ 2100 mm yr-1的应用条件下模型参数误差所导致不确定性区间为±3.2%。统计建模所采用DNDC蒙特卡洛数据样本,经点位验证DNDC模拟值与实测报道值相对偏差、均方根误差分别为+10.2%、1.7；最优排放模型评估结果的交叉验证R2为0.845,其表现优于同类研究。我国毛竹林施肥N2O排放,随施肥量增长而呈上升态势,自第一次全国森林资源清查以来的40年内,毛竹林N2O排放总量从1973年的16±0.3 Gg yr-1升至2012年的17.0±3.6Gg yr-1,年均增长率达6.2%；降水量是主要活性氮源强调控因子,导致肥料氮至N2O转化足迹的地域差异,内陆省份单位施肥量所致N2O排放较沿海地区高38.0%。(2)化石燃料燃烧的NOx排放与夜间灯光强度显著相关。经聚类分析比选,建立了DMSP/OLS夜间稳定灯光遥感影像栅格单位灰度值NOx排放的分区指标,将研究区内30省划分为Ⅰ区和Ⅱ区,Ⅰ区包括内蒙古、江西、湖北、湖南、四川与贵州6省、Ⅱ区包括北京、上海、广东等其余24省和自治区；NOx排放最优评估模型分别为Ⅰ区y=1.070x(R2=0.948),Ⅱ区y=0.696x(R2=0.950),其中y为NOx排放源强、x为DMSP/OLS夜间稳定灯光遥感影像栅格灰度值；灯光模型评估结果与已有清单、遥感反演结果具有较高可比性,NOx年排放评估值较清单文献值高4.1%-13.8%,NOx排放强度与对流层NO2垂直柱浓度遥感反演数据相关系数为0.740-0.794(p0.01)。基于我国在“九五”至“十一五”期间可获取的DMSP/OLS数据,计算了化石燃料燃烧的NOx排放,结果显示NOx排放从1995年的8.6 Tg增长至2010年的28.1 Tg,年均增长率达8.2%；全国NOx排放强度的Moran's Ⅰ指数在研究期内增长50.7%,表明NOx排放空间集聚性逐年增强,其中京津冀、长三角、珠三角地区呈典型高-高集聚特征,对周边区域NOx排放具有强大的辐射与带动作用。(3)经N2O与NOx足迹分析,提出了大气氮排放的空间分异管控措施。对农业毛竹林N2O排放,经情景模拟足迹分析,沿海地区首要控制施肥方式,内陆地区则首要控制肥料种类,将在不影响毛竹产量的前提下使我国毛竹林N2O减排潜力于2030年达11.1 Tg yr-1 CO2-eq,其减排量约为当前我国农田N2O总排放量的5.6%。对化石燃料燃烧NOx排放,经区域间投入产出分析,NOx排放热区京津、南部沿海、东部沿海地区因对外部进口商品与服务消费分别产生127.4、631.4、697.2Ggyr-1隐含氮足迹(以NOx计),在生产型NOx减排管理的同时加强对该区域低氮消费模式的引导可有效降低全国氮足迹。
[Abstract]:The disturbance of human activity to natural nitrogen cycle leads to a sharp increase in the emission of active nitrogen atmosphere. It is of great significance to clarify the spatial and temporal pattern of its emission. The ratio of agricultural production and fossil fuel combustion to the anthropogenic atmospheric active nitrogen emissions in the world is 56.5% and 35.3%, respectively. The greenhouse gas Nitrous Oxide (N20) from agricultural fertilization and the two fine particulate matter precursor nitrogen oxides (NOx) from fossil fuels are typical pollutants in the emission of active nitrogen. However, due to the lack of spatial data, the assessment of the spatial distribution of N20 and NOx emission sources is still quite challenging. The development of remote sensing technology provides spatial information for the assessment of active nitrogen space, but it is not clear how to excavate spatial information data and then quantify the temporal and spatial regularity of active nitrogen emission. This paper aims to use multi source data and statistical modeling methods from the perspective of biogeochemistry and human activity footprint of active nitrogen in different time and region. Solve the problem of data lack, analyze the spatial and temporal pattern of N20 and fossil fuel combustion NOx emission. On the basis of the emission list, the biogeochemical model and the remote sensing inversion method, the largest data can be taken as the time boundary with the provinces and cities in China as the spatial scale, and the literature data and all the papers are studied through the statistical yearbook. The data sharing platform of the ball remote sensing data sharing platform is used to study the N20 emission of agricultural fertilization and the time and space Footprint Assessment Model of the NOx emission from fossil fuel combustion. Taking the typical typical economic crop of Mao bamboo in our country, using the biogeochemical process model DeComposition-DeNitrification (DNDC) Monte Carlo simulation data samples, the partial correlation is divided into the partial correlation. The evaluation parameters were selected, and the N20 emission model was constructed by stepwise multiple regression analysis, and the strong distribution of N20 emission source in the bamboo forest in China was evaluated. The regional division based on the cluster analysis was carried out through the correlation analysis of the DMSP/OLS night stable light remote sensing data and the NOx emission. The domain based on the night light based NOx emission regression model, and using the Moran's1 index based on spatial autocorrelation analysis to analyze the spatial agglomeration characteristics of NOx emissions, and to explore the management countermeasures of the N20 and NOx footprints through the analysis of agricultural fertilization scenarios and the multi regional input and output analysis of the hidden nitrogen footprint of regional trade circulation. The following conclusions are as follows: (1) the spatio-temporal pattern of Mao Zhulin's fertilized active nitrogen N20 emission (E) is significantly related to nitrogen fertilizer application (N) and precipitation (P). The optimal emission assessment model is E=0.057 N-2.61 x 10-3P, and the optimal emission assessment model is E=0.057 N-2.61 x 10-3P, and is 96 less than N < 298 kgN hm-2700 < P < 2100. DNDC Monte Carlo data samples are used in the uncertain interval of the model parameter error of the model under the application conditions, and the relative deviation between the DNDC simulation value and the measured report value is verified by point position, and the root mean square error is +10.2%, 1.7 respectively. The cross validation of the optimal emission model evaluation results is 0.845, and its performance is better than that of the same kind of research. The N2O emission of bamboo forest in China is rising with the increase of fertilization. In 40 years since the first national forest resource inventory, the total N2O emission of bamboo forest has risen from 16 + 0.3 Gg yr-1 in 1973 to 17 + 3.6Gg yr-1 in 2012, with an annual average growth rate of 6.2%; precipitation is the main active nitrogen source which emphasizes control factors, leading to fertilizer nitrogen to N2 The regional difference of the O conversion footprint, the N2O emission from the inland province, the higher 38.0%. (2) than the coastal area, the NOx emission from the combustion of fossil fuel is significantly related to the night light intensity. By cluster analysis, the zoning index of NOx emission of the grid unit grey degree of DMSP/OLS at night stable light remote sensing image is established, and the 30 provinces in the study area will be set up. The area I was divided into area I and II, including Inner Mongolia, Jiangxi, Hubei, Hunan, Sichuan and Guizhou, the other 24 provinces and autonomous regions, including Beijing, Shanghai, Guangdong, and other 24 provinces and autonomous regions; NOx emission optimal evaluation model was I region y=1.070x (R2=0.948), and II zone y=0.696x (R2= 0.950), of which y was NOx emission source, X was DMSP/OLS night stable light remote sensing The gray value of the image grid, the evaluation results of the light model and the existing list, the remote sensing inversion results have high comparability. The NOx emission assessment value is higher than the list literature value 4.1%-13.8%. The correlation coefficient of the NOx emission intensity and the remote sensing inversion data of the vertical column concentration of the troposphere is 0.740-0.794 (P0.01). Based on our country from "95" to "11th Five-Year" The available DMSP/OLS data calculated the NOx emission of fossil fuel combustion. The results showed that the NOx emission increased from 8.6 Tg in 1995 to 28.1 Tg in 2010, and the annual growth rate was 8.2%. The Moran's I index of national NOx emission intensity increased by 50.7% in the study period, indicating that the spatial agglomeration of NOx emissions increased year by year, including Beijing, Tianjin Hebei, and long three. Angle, the Pearl River Delta region has a typical high concentration characteristic, which has strong radiation and driving effect on the NOx emission in the surrounding region. (3) the spatial differentiation and control measures for atmospheric nitrogen emissions are proposed by N2O and NOx footprint analysis. The agricultural Mao Zhulin N2O emission, the scene simulation footprint analysis, the primary control fertilization mode in the coastal areas, and the inland areas The primary control of the type of fertilizer will make the N2O emission reduction potential of the bamboo forest in China up to 11.1 Tg yr-1 CO2-eq in 2030 without affecting the yield of bamboo, and its reduction is about NOx emission from the current N2O total emission of farmland by 5.6%. to fossil fuels, through the interregional input and output analysis, the NOx emission heat area, the southern coast and the east coast. In the region, the 127.4631.4697.2Ggyr-1 hidden nitrogen footprint (NOx) is produced for the external import goods and service consumption, and the guidance of the low nitrogen consumption pattern in the region can effectively reduce the national nitrogen footprint in the management of the production type NOx emission reduction.
【学位授予单位】：浙江大学
【学位级别】：博士
【学位授予年份】：2016
【分类号】：X511

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