氧化亞氮與氮氧化物時空足跡模型研究
本文選題:農業(yè)施肥 + 化石燃料燃燒。 參考:《浙江大學》2016年博士論文
【摘要】:人類活動對自然氮循環(huán)過程的擾動導致活性氮大氣排放急劇增長,明確其排放時空格局對氣候變化減緩以及相應大氣污染控制措施的制定具有重要意義。農業(yè)生產與化石燃料燃燒在全球人為大氣活性氮排放中占比分別為56.5%、35.3%;我國來自農業(yè)施肥的溫室氣體氧化亞氮(N20)和來自化石燃料燃燒的二次細顆粒物主要前體物氮氧化物(NOx)是活性氮排放中的典型污染物。然而,由于空間數據的缺乏,N20和NOx排放源強的空間分布評估仍頗具挑戰(zhàn)。生物地球化學過程模型、遙感技術的發(fā)展為活性氮空間評估提供了空間信息,但如何挖掘空間信息數據,進而量化活性氮排放時空規(guī)律,目前尚不明確。本文旨在從活性氮在不同時間與地域的生物地球化學與人類活動足跡視角,利用多源數據與統(tǒng)計建模手段破解數據缺乏難題,解析農業(yè)施肥N20與化石燃料燃燒NOx排放時空格局。在排放清單、生物地球化學模型與遙感反演方法綜述基礎上,以中國省市區(qū)域為空間尺度、最大數據可獲取年份為時間邊界,通過統(tǒng)計年鑒、研究論文等文獻數據與全球遙感數據共享平臺數據采集,研究了農業(yè)施肥的N20排放與化石燃料燃燒的NOx排放時空足跡評估模型。以我國典型特色經濟作物毛竹為例,利用生物地球化學過程模型DeComposition-DeNitrification (DNDC)蒙特卡洛模擬數據樣本,通過偏相關分析法篩選評估參數,進而采用逐步多元回歸分析法構建了施肥N20排放計算模型,評估我國省域尺度毛竹林N20排放源強分布;通過DMSP/OLS夜間穩(wěn)定燈光遙感數據與NOx排放相關性分析驗證,開展了基于聚類分析的地域分區(qū),構建了不同區(qū)域基于夜間燈光的燃燒源NOx排放回歸模型,并采用基于空間自相關分析的Moran's1指數解析了NOx排放的空間集聚特征;通過農業(yè)施肥情景分析與區(qū)域問貿易流通隱含氮足跡的多區(qū)域投入產出分析探討了N20與NOx足跡的管理對策。主要研究結論如下:(1)毛竹林施肥活性氮N20排放(E)時空格局與氮肥施用量(N)和降水量(P)顯著相關。比選三種基于當前施肥N20排放影響理論的線性與非線性模型,最優(yōu)排放評估模型為E=0.057 N-2.61×10-3P,在 96≤N≤298 kgN hm-2、700≤P≤ 2100 mm yr-1的應用條件下模型參數誤差所導致不確定性區(qū)間為±3.2%。統(tǒng)計建模所采用DNDC蒙特卡洛數據樣本,經點位驗證DNDC模擬值與實測報道值相對偏差、均方根誤差分別為+10.2%、1.7;最優(yōu)排放模型評估結果的交叉驗證R2為0.845,其表現優(yōu)于同類研究。我國毛竹林施肥N2O排放,隨施肥量增長而呈上升態(tài)勢,自第一次全國森林資源清查以來的40年內,毛竹林N2O排放總量從1973年的16±0.3 Gg yr-1升至2012年的17.0±3.6Gg yr-1,年均增長率達6.2%;降水量是主要活性氮源強調控因子,導致肥料氮至N2O轉化足跡的地域差異,內陸省份單位施肥量所致N2O排放較沿海地區(qū)高38.0%。(2)化石燃料燃燒的NOx排放與夜間燈光強度顯著相關。經聚類分析比選,建立了DMSP/OLS夜間穩(wěn)定燈光遙感影像柵格單位灰度值NOx排放的分區(qū)指標,將研究區(qū)內30省劃分為Ⅰ區(qū)和Ⅱ區(qū),Ⅰ區(qū)包括內蒙古、江西、湖北、湖南、四川與貴州6省、Ⅱ區(qū)包括北京、上海、廣東等其余24省和自治區(qū);NOx排放最優(yōu)評估模型分別為Ⅰ區(qū)y=1.070x(R2=0.948),Ⅱ區(qū)y=0.696x(R2=0.950),其中y為NOx排放源強、x為DMSP/OLS夜間穩(wěn)定燈光遙感影像柵格灰度值;燈光模型評估結果與已有清單、遙感反演結果具有較高可比性,NOx年排放評估值較清單文獻值高4.1%-13.8%,NOx排放強度與對流層NO2垂直柱濃度遙感反演數據相關系數為0.740-0.794(p0.01)。基于我國在“九五”至“十一五”期間可獲取的DMSP/OLS數據,計算了化石燃料燃燒的NOx排放,結果顯示NOx排放從1995年的8.6 Tg增長至2010年的28.1 Tg,年均增長率達8.2%;全國NOx排放強度的Moran's Ⅰ指數在研究期內增長50.7%,表明NOx排放空間集聚性逐年增強,其中京津冀、長三角、珠三角地區(qū)呈典型高-高集聚特征,對周邊區(qū)域NOx排放具有強大的輻射與帶動作用。(3)經N2O與NOx足跡分析,提出了大氣氮排放的空間分異管控措施。對農業(yè)毛竹林N2O排放,經情景模擬足跡分析,沿海地區(qū)首要控制施肥方式,內陸地區(qū)則首要控制肥料種類,將在不影響毛竹產量的前提下使我國毛竹林N2O減排潛力于2030年達11.1 Tg yr-1 CO2-eq,其減排量約為當前我國農田N2O總排放量的5.6%。對化石燃料燃燒NOx排放,經區(qū)域間投入產出分析,NOx排放熱區(qū)京津、南部沿海、東部沿海地區(qū)因對外部進口商品與服務消費分別產生127.4、631.4、697.2Ggyr-1隱含氮足跡(以NOx計),在生產型NOx減排管理的同時加強對該區(qū)域低氮消費模式的引導可有效降低全國氮足跡。
[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.
【學位授予單位】:浙江大學
【學位級別】:博士
【學位授予年份】:2016
【分類號】:X511
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