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1.
Impacts of atmospheric anthropogenic nitrogen on the open ocean 总被引：3，自引：0，他引：3
Duce RA LaRoche J Altieri K Arrigo KR Baker AR Capone DG Cornell S Dentener F Galloway J Ganeshram RS Geider RJ Jickells T Kuypers MM Langlois R Liss PS Liu SM Middelburg JJ Moore CM Nickovic S Oschlies A Pedersen T Prospero J Schlitzer R Seitzinger S Sorensen LL Uematsu M Ulloa O Voss M Ward B Zamora L 《Science (New York, N.Y.)》2008,320(5878):893-897
Increasing quantities of atmospheric anthropogenic fixed nitrogen entering the open ocean could account for up to about a third of the ocean's external (nonrecycled) nitrogen supply and up to approximately 3% of the annual new marine biological production, approximately 0.3 petagram of carbon per year. This input could account for the production of up to approximately 1.6 teragrams of nitrous oxide (N2O) per year. Although approximately 10% of the ocean's drawdown of atmospheric anthropogenic carbon dioxide may result from this atmospheric nitrogen fertilization, leading to a decrease in radiative forcing, up to about two-thirds of this amount may be offset by the increase in N2O emissions. The effects of increasing atmospheric nitrogen deposition are expected to continue to grow in the future. 相似文献
2.
Nitrous oxide (N(2)O) and methane (CH(4)) are chemically reactive greenhouse gases with well-documented atmospheric concentration increases that are attributable to anthropogenic activities. We quantified the link between N(2)O and CH(4) emissions through the coupled chemistries of the stratosphere and troposphere. Specifically, we simulated the coupled perturbations of increased N(2)O abundance, leading to stratospheric ozone (O(3)) depletion, altered solar ultraviolet radiation, altered stratosphere-to-troposphere O(3) flux, increased tropospheric hydroxyl radical concentration, and finally lower concentrations of CH(4). The ratio of CH(4) per N(2)O change, -36% by mole fraction, offsets a fraction of the greenhouse effect attributable to N(2)O emissions. These CH(4) decreases are tied to the 108-year chemical mode of N(2)O, which is nine times longer than the residence time of direct CH(4) emissions. 相似文献
3.
Measurements of the oxygen isotope ratios (18O/16O and 17O/16O) in atmospheric nitrous oxide (N2O) from La Jolla, Pasadena, and the White Mountain Research Station (elevation, 3801 meters) in California and the White Sands Missile Range in New Mexico show that N2O has a mass-independent composition. These data suggest the presence of a previously undefined atmospheric process. The La Jolla samples can be explained by a mixing between an atmospherically derived source of mass-independent N2O and biologically derived mass-dependent N2O. Possible origins of the mass-independent anomaly in N2O are discussed. 相似文献
4.
PO Wennberg TF Hanisco L Jaegle DJ Jacob EJ Hintsa EJ Lanzendorf JG Anderson R Gao ER Keim SG Donnelly LAD Negro DW Fahey SA McKeen RJ Salawitch CR Webster RD May RL Herman MH Proffitt JJ Margitan EL Atlas SM Schauffler F Flocke CT McElroy TP Bui 《Science (New York, N.Y.)》1998,279(5347):49-53
The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HOx required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of O3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more O3 than expected. 相似文献
5.
Nitrous oxide in the earth's atmosphere contributes to catalytic stratospheric ozone destruction and is also a greenhouse gas component. A precise budgetary accounting of N(2)O sources has remained elusive, and there is an apparent lack of source identification. One source of N(2)O is as a by-product in the manufacture of nylon, specifically in the preparation of adipic acid. Characterization of the reaction N(2)O stoichiometry and its isotopic composition with a simulated industrial adipic acid synthesis indicates that because of high rates of global adipic acid production, this N(2)O may account for approximately 10 percent of the increase observed for atmospheric N(2)O. 相似文献
6.
对大气中气相氮化合物的源汇状况及其引起的气候和环境效应进行了较为详尽的综述： 分析了大气温室气体Ｎ２ Ｏ 及影响大气质量和环境的含氮化合物ＮＯｘ 的源汇种类及强度;对含氮化合物在大气中的各种化学反应过程作了综合剖析;针对与农业过程密切相关的生物源－ 土壤中由微生物参与的硝化作用与反硝化作用过程与机制及其产生气相氮化物的可能路径和主要影响因子进行了详细分析; 并提出了减少排放与控制的措施和途径。 相似文献
7.
The results of an analysis of more than 60,000 atmospheric measurements of carbon monoxide taken over 3(1/2) years at Cape Meares, Oregon (45 degrees N, 125 degrees W), indicate that the background concentration of this gas is increasing. The rate of increase, although uncertain, is about 6 percent per year on average. Human activities are the likely cause of a substantial portion of this observed increase; however, because of the short atmospheric lifetime of carbon monoxide and the relatively few years of observations, fluctuations of sources and sinks related to the natural variability of climate may have affected the observed trend. Increased carbon monoxide may deplete tropospheric hydroxyl radicals, slowing down the removal of dozens of man-made and anthropogenic trace gases and thus indirectly affecting the earth's climate and possibly the stratospheric ozone layer. 相似文献
8.
Brune WH Toohey DW Anderson JG Starr WL Vedder JF Danielsen EF 《Science (New York, N.Y.)》1988,242(4878):558-562
In order to test photochemical theories linking chlorofluorocarbon derivatives to ozone(O(3)) depletion at high latitudes in the springtime, several related atmospheric species, including O(3), chlorine monoxide(ClO), and bromine monoxide (BrO) were measured in the lower stratosphere with instruments mounted on the NASA ER-2 aircraft on 13 February 1988. The flight path from Moffett Field, California (37 degrees N, 121 degrees W), to Great Slave Lake, Canada (61 degrees N, 115 degrees W), extended to the center of the polar jet associated with but outside of the Arctic vortex, in which the abundance of O(3) was twice its mid-latitude value, whereas BrO levels were 5 parts per trillion by volume (pptv) between 18 and 21 kilometers, and 2.4 pptv below that altitude. The ClO mixing ratio was as much as 65 pptv at 60 degrees N latitude at an altitude of 20 kilometers, and was enhanced over mid-latitude values by a factor of 3 to 5 at altitudes above 18 kilometers and by as much as a factor of 40 at altitudes below 17 kilometers. Levels of ClO and O(3) were highly correlated on all measured distance scales, and both showed an abrupt change in character at 54 degrees N latitude. The enhancement of ClO abundance north of 54 degrees N was most likely caused by low nitrogen dioxide levels in the flight path. 相似文献
9.
从2000年9月到2001年9月,每月两次采样连续监测太湖地区湖、河和井水水体中溶解的N2O浓度、NO-3-N和NH4+-N浓度及水温的变化,研究了湖、河、井水体NO-3-N和NH4+-N浓度对水中溶解N2O浓度的影响。结果表明,湖、河和井水中溶解的N2O浓度与NO-3-N浓度呈显著正相关关系,也与水温呈正相关,而与NH4+-N浓度无显著相关关系。结果还表明,浅水型水体高浓度NO-3-N和NH4+-N的存在均是N2O产生的源;水体反硝化作用和硝化-反硝化均是水中产生N2O的重要途径。 相似文献
10.
The ocean is an important global source of nitrous oxide (N(2)O), a greenhouse gas that contributes to stratospheric ozone destruction. Bacterial nitrification and denitrification are thought to be the primary sources of marine N(2)O, but the isotopic signatures of N(2)O produced by these processes are not consistent with the marine contribution to the global N(2)O budget. Based on enrichment cultures, we report that archaeal ammonia oxidation also produces N(2)O. Natural-abundance stable isotope measurements indicate that the produced N(2)O had bulk δ(15)N and δ(18)O values higher than observed for ammonia-oxidizing bacteria but similar to the δ(15)N and δ(18)O values attributed to the oceanic N(2)O source to the atmosphere. Our results suggest that ammonia-oxidizing archaea may be largely responsible for the oceanic N(2)O source. 相似文献
11.
Paleoatmospheric records of trace-gas concentrations recovered from ice cores provide important sources of information on many biogeochemical cycles involving carbon, nitrogen, and oxygen. Here, we present a 106,000-year record of atmospheric nitrous oxide (N2O) along with corresponding isotopic records spanning the last 30,000 years, which together suggest minimal changes in the ratio of marine to terrestrial N2O production. During the last glacial termination, both marine and oceanic N2O emissions increased by 40 +/- 8%. We speculate that our records do not support those hypotheses that invoke enhanced export production to explain low carbon dioxide values during glacial periods. 相似文献
12.
Convective updrafts in thunderstorms prolong the lifetime of ozone (O(3)) and its anthropogenic precursor NOx [nitric oxide (NO) + nitrogen dioxide (NO(2))] by carrying these gases rapidly upward from the boundary layer into a regime where the O(3) production efficiency is higher, chemical destruction is slower, and surface deposition is absent. On the other hand, the upper troposphere is relatively rich in O(3) and NOx from natural sources such as downward transport from the stratosphere and lightning; convective overturning conveys the O(3) and NOx toward the Earth's surface where these components are more efficiently removed from the atmosphere. Simulations with a three-dimensional global model suggest that the net result of these counteractive processes is a 20 percent overall reduction in total tropospheric O(3). However, the net atmospheric oxidation efficiency is enhanced by 10 to 20 percent. 相似文献
13.
The reactions of dinitrogen pentoxide (N(2)O(5)) with H(2)O and hydrochloric acid (HCl) were studied on ice surfaces in a Knudsen cell flow reactor. The N(2)O(5) reacted on ice at 185 K to form condensed-phase nitric acid (HNO(3)). This reaction may provide a sink for odd nitrogen (NO(x)) during the polar winter, a requirement in nearly all models of Antarctic ozone depletion. A lower limit to the sticking coefficient, gamma, for N(2)O(5) on ice is 1 x 10(-3). Moreover, N(2)O(5) reacted on HCl-ice surfaces at 185 K, with gamma greater than 3 x 10(-3). This reaction, which produced gaseous nitryl chloride (ClNO(2)) and condensed-phase HNO(3), proceeded until all of the HCl within the ice was depleted. The ClNO(2), which did not react or condense on ice at 185 K, can be readily photolyzed in the Antarctic spring to form atomic chlorine for catalytic ozone destruction cycles. The other photolysis product, gaseous nitrogen dioxide (NO(2)), may be important in the partitioning of NO(x) between gaseous and condensed phases in the Antarctic winter. 相似文献
14.
Miller RL Suits AG Houston PL Toumi R Mack JA Wodtke AM 《Science (New York, N.Y.)》1994,265(5180):1831-1838
Highly vibrationally excited O(2)(X(3)sigmag(-), v >/= 26) has been observed from the photodissociation of ozone (O(3)), and the quantum yield for this reaction has been determined for excitation at 226 nanometers. This observation may help to address the "ozone deficit" problem, or why the previously predicted stratospheric O(3) concentration is less than that observed. Recent kinetic studies have suggested that O(2)(X(3)sigmag(-), v >/= 26) can react rapidly with O(2) to form O(3) + O and have led to speculation that, if produced in the photodissociation of O(3), this species might be involved in resolving the discrepancy. The sequence O(3) + hv --> O(2)(X(3)sigmag(-), v >/= 26) + O; O(2)(X(3)sigmag(-), v >/= 26) + O(2) --> O(3) + O (where hv is a photon) would be an autocatalytic mechanism for production of odd oxygen. A two-dimensional atmospheric model has been used to evaluate the importance of this new mechanism. The new mechanism can completely account for the tropical O(3) deficit at an altitude of 43 kilometers, but it does not completely account for the deficit at higher altitudes. The mechanism also provides for isotopic fractionation and may contribute to an explanation for the anomalously high concentration of heavy O(3) in the stratosphere. 相似文献
15.
The global budget of N(2)O shows a significant imbalance between the known rate of destruction in the stratosphere and the estimated rates of natural and anthropogenic production in soils and the ocean. Measurements of the (15)N/(14)N and (18)O/(16)O ratios in two major tropospheric sources of N(2)O, tropical rain forest soils and fertilized soils, show that soil N(2)O from a tropical rain forest in Costa Rica and from sugar-cane fields in Maui is strongly depleted in both (15)N and (18)O relative to mean tropospheric N(2)O. A major source of heavy N(2)O, enriched in both (15)N and (18)O, must therefore be present to balance the light N(2)O from soils. One such source is the back-mixing flux of N(2)O from the stratosphere, which is enriched in (15)N and (18)O by photolysis and chemistry. However these return fluxes of (15)N and (18)O are so great that a large oceanic flux of N(2)O is required to balance the heavy isotope-enriched stratospheric flux. All these effects will be reflected in climatically related isotopic variations in trapped N(2)O in polar ice cores. 相似文献
16.
崇明岛稻麦轮作系统稻田温室气体排放研究 总被引：7，自引：3，他引：4
通过静态箱-气相色谱法,研究了崇明岛稻麦轮作地水稻生长季及收割后休耕期(2011年6月至2011年11月)温室气体CO2、CH4和N2O的排放、吸收规律及交换量,并运用增温潜势进行了温室效应估算。3种温室气体通量在水稻不同生长阶段有明显差异:稻田除成熟收割期外,其他期均表现为CH4排放源,并在分蘖期达到最大值;N2O除幼苗期表现为汇,其他期均为排放源,并在拔节期达到最大值。温室效应分析得出:水稻田温室气体以CH4和N2O排放为主,二者对全球温室效应的贡献为3.255×103kgCO2·hm-2;由于光合作用,稻田表现为对CO2固定,固定量为2.462×103kgCO·2hm-2;崇明水稻生长季排放温室气体综合GWP值为793kgCO·2hm-2,为温室气体排放源。 相似文献
17.
18.
Brown SS Ryerson TB Wollny AG Brock CA Peltier R Sullivan AP Weber RJ Dubé WP Trainer M Meagher JF Fehsenfeld FC Ravishankara AR 《Science (New York, N.Y.)》2006,311(5757):67-70
Nitrogen oxides in the lower troposphere catalyze the photochemical production of ozone (O3) pollution during the day but react to form nitric acid, oxidize hydrocarbons, and remove O3 at night. A key nocturnal reaction is the heterogeneous hydrolysis of dinitrogen pentoxide, N2O5. We report aircraft measurements of NO3 and N2O5, which show that the N2O5 uptake coefficient, g(N2O5), on aerosol particles is highly variable and depends strongly on aerosol composition, particularly sulfate content. The results have implications for the quantification of regional-scale O3 production and suggest a stronger interaction between anthropogenic sulfur and nitrogen oxide emissions than previously recognized. 相似文献
19.
The atmospheric residence time for methyl bromide (CH3Br) has been estimated as 0.8 +/- 0.1 years from its empirical spatial variability relative to C2H6, C2Cl4, CHCl3, and CH3Cl. This evaluation of the atmospheric residence time, based on Junge's 1963 general proposal, provides an estimate for CH3Br that is independent of source and sink estimates. Methyl bromide from combined natural and anthropogenic sources furnishes about half of the bromine that enters the stratosphere, where it plays an important role in ozone destruction. This residence time is consistent with the 0.7-year value recently calculated for CH3Br from the combined strength estimates for its known significant sinks. 相似文献
20.
Nitrous oxide, methane, ammonia, and a number of other trace constituents in the earth's atmosphere have infrared absorption bands in the spectral region 7 to 14 microm and contribute to the atmospheric greenhouse effect. The concentrations of these trace gases may undergo substantial changes because of man's activities. Extensive use of chemical fertilizers and combustion of fossil fuels may perturb the nitrogen cycle, leading to increases in atmospheric N(2)O, and the same perturbing processes may increase the amounts of atmospheric CH(4) and NH(3). We use a one-dimensional radiative-convective model for the atmospheric thermal structure to compute the change in the surface temperature of the earth for large assumed increases in the trace gas concentrations; doubling the N(2)O, CH(4), and NH(3) concentrations is found to cause additive increases in the surface temperature of 0.7 degrees , 0.3 degrees , and 0.1 degrees K, respectively. These systematic effects on the earth's radiation budget would have substantial climatic significance. It is therefore important that the abundances of these trace gases be accurately monitored to determine the actual trends of their concentrations. 相似文献