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1.
Recently, additional ozone production mechanisms have been proposed to resolve the ozone deficit problem, which arises from greater ozone destruction than production in several photochemical models of the upper stratosphere and lower mesosphere. A detailed ozone model budget analysis was performed with simultaneous observations of O(3), HCl, H(2)O, CH(4), NO, and NO(2) from the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS) under conditions with the strongest photochemical control of ozone. The results indicate that an ozone deficit may not exist. On the contrary, the use of currently recommended photochemical parameters leads to insufficient ozone destruction in the model.  相似文献   

2.
Chain decomposition of ozone by hydroxyl and hydroperoxyl radicals has been observed. The rate constant at 3000 degrees K for OH + O(3)-->HO(2) + O(2) is 8 x 10(-14) cubic centimeters per second. The rate constant for HO(2) + O(3)--> OH + 2O(2), is 3 x 10(-15) cubic centimeters per second. These results have implications concerning stratospheric ozone.  相似文献   

3.
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   

4.
The elusive protonated ozone ion (O(3)H(+)) has been long postulated as a reactive intermediate but never experimentally observed. This ion has been detected here in mass spectrometric experiments with the use of Fourier transform ion cyclotron resonance. In these experiments, ozone (O(3)) was protonated by strong acids-for example, H(3)(+), KrH(+), XeH(+), and CH(5)(+). The hitherto experimentally unknown proton affinity of O(3) was evaluated by a "bracketing" technique and determined to be 148 -/+ 3 kilocalories mole(-1) at 298 kelvin, in excellent agreement with a value determined in a recent theoretical study of the O(3)/O(3)H(+) system, which was 148 kilocalories mole(-1) at zero temperature ( approximately 149.5 kilocalories mole(-1) at 298 kelvin).  相似文献   

5.
GI Gellene 《Science (New York, N.Y.)》1996,274(5291):1344-1346
Application of a theory of nuclear symmetry-based reaction restrictions to the O2 + O --> O3 reaction provides a potential explanation for the symmetry-induced isotopic enrichment observed for laboratory and atmospherically produced O3. Within this theory, the rate of formation of O3 from collisions of O and isotopically homonuclear O2 depends on whether the O2 molecule is in an f (allowed) or an e (restricted) parity label state. The restriction can be relaxed by various potential energy surface coupling terms, and the assumption that approximately 78 percent of the restricted O2(e) levels produce O3 with the same efficiency as the allowed O2(f) levels can account for laboratory-observed isotopic fractionation. In particular, the theory explains the special enhanced formation of the completely asymmetric isotopomer 16O17O18O.  相似文献   

6.
From measurements of the photochemical rate of production of CO(2)(16,18) and CO(2)(16,16), produced from the low intensity photolysis of mixtures of CO, H(2)O, Ar, and O(2)(18,18), the rate constant for the reaction HO(2) + CO --> CO(2) + OH has been determined at 300 degrees K to be less than or equal to 10(-20) cubic centimeter per molecule per second. These measurements indicate that the reaction of thermalized HO(2) is of negligible importance as a sink mechanism for converting CO to CO(2) in either the troposphere or the stratosphere.  相似文献   

7.
A comprehensive inelastic neutron scattering study of magnetic excitations in the near optimally doped high-temperature superconductor YBa(2)Cu(3)O(6.85) is presented. The spin correlations in the normal state are commensurate with the crystal lattice, and the intensity is peaked around the wave vector characterizing the antiferromagnetic state of the insulating precursor, YBa(2)Cu(3)O(6). Profound modifications of the spin excitation spectrum appear abruptly below the superconducting transition temperature T(c), where a commensurate resonant mode and a set of weaker incommensurate peaks develop. The data are consistent with models that are based on an underlying two-dimensional Fermi surface, predicting a continuous, downward dispersion relation connecting the resonant mode and the incommensurate excitations. The magnetic incommensurability in the YBa(2)Cu(3)O(6+)(x) system is thus not simply related to that of another high-temperature superconductor, La(2-)(x)Sr(x)CuO(4), where incommensurate peaks persist well above T(c). The temperature-dependent incommensurability is difficult to reconcile with interpretations based on charge stripe formation in YBa(2)Cu(3)O(6+x) near optimum doping.  相似文献   

8.
臭氧胁迫对水稻光合作用与产量的影响   总被引：3，自引：1，他引：2  
采用开顶式气室(OTC),对水稻"3694繁"(Oryza sativa L.3694 Fan)进行田间原位臭氧(O_3)熏气实验,研究了不同O_3浓度熏气处理下水稻光合色素、气体交换参数以及产量的响应.实验设置分4个水平:过滤大气组(CF,10 nL·L~(-1))、自然大气组(NF,40nL·L~(-1))和两个不同浓度的O_3处理组(01:100 nL·L~(-1);02:150 nL·L~(-1)).结果表明:(1)与CF组相比,两个不同浓度的O_3处理均导致水稻叶片光合色素含量大幅度下降,加速水稻的衰老过程;(2)在实验进程中,O_3处理导致水稻叶片气体交换参数发生显著变化,饱和CO:浓度的净光合速率(P_(sat))、气孔导度(Gs)、水分利用效率(WUE)、气孔限制值(Ls)和羧化效率(CE)均呈现下降趋势,表明O,浓度的升高使水稻光合作用对CO_2的利用效率降低,水稻在灌浆期对O_3最为敏感;(3)O_3处理使水稻产量损失明显,当AOT40值达到2.32uL·L~(-1)·h时,就能导致水稻产量10%的减产.  相似文献   

9.
紫色马铃薯“3414”肥效研究   总被引：1，自引：0，他引：1  
[目的]为解决生产上存在的盲目和过度施肥现象,提高肥料利用率。[方法]以紫色马铃薯材料KX-5为试材,采用"3414"完全实施方案设计,研究了西南二季作区春季紫色马铃薯的施肥模式。[结果]紫色马铃薯产量(Y)与肥料水平(X1-N,X2-P2O5,X3-K2 O)的最优三元二次肥料效应函数方程为Y=1 352.67-89.78X1+14.17X2+144.98X3-8.03X1 2-5.07X2 2-3.83X3 2+36.46X1 X2-2.54X1 X3-12.95X2 X3,获得最佳产量的氮、磷、钾施肥量为61.80、73.65、131.25 kg/hm2。[结论]该研究可用来指导当地紫薯生产经济施肥。  相似文献   

10.
Triclinic ulexite crystals contain isolated borate polyanions [B(5)O(6)(OH)(6)](3-) related to the well known pentaborate polyanion [B(5)O(6)(OH)(4)](-) by addition of two hydroxyl groups to two opposite B-O triangles. The isolated ulexite polyanions form the [B(5)O(7)(OH)(4)](n)(3n-) chains previously found in crystals of the related mineral probertite, NaCaB(5)O(7)(OH)(4).3H(2)O.  相似文献   

11.
Chlorine nitrate photolysis has been investigated with the use of a molecular beam technique. Excitation at both 248 and 193 nanometers led to photodissociation by two pathways, CIONO(2) --> CIO + NO()2 and CIONO(2) --> Cl + NO3, with comparable yields. This experiment provides a direct measurement of the CIO product channel and consequently raises the possibility of an analogous channel in CIO dimer photolysis. Photodissociation of the CIO dimer is a critical step in the catalytic cycle that is presumed to dominate polar stratospheric ozone destruction. A substantial yield of CIO would reduce the efficiency of this cycle.  相似文献   

12.
基于树干液流技术对杨树冠层吸收臭氧特征的分析1）   总被引：1，自引：0，他引：1  
基于树干液流的技术方法,在自然状态下对杨树（ Populus spp．）臭氧吸收特征进行了研究。结果表明：臭氧质量浓度日变化呈单峰型,其变化范围为25．5～175．0μg· m－3;臭氧吸收速率（ FO3）和臭氧吸收导度（ GO3）日变化均为单峰型;FO3均值为（78．22±39．45）nmol· m－2· s－1,GO3均值为（127．60±64．35）mmol· m－2· s－1;环境因子水汽压亏缺（D）、太阳辐射（Rs）和风速对FO3和GO3的响应,导致臭氧吸收通量相对较高,D对更高的GO3和FO3更敏感,随着D增加臭氧吸收减少,Rs在达到50 W· m－2时GO3和FO3也有所降低;臭氧质量浓度抑制树木蒸腾,影响液流密度的变化;臭氧质量浓度超过临界水平引起树木相应的响应,杨树AOT40为72．02 mg· m－3· h－1,远超过对树木危害的臭氧质量浓度的临界水平10．71 mg· m－3· h－1,说明了杨树的高臭氧风险,树干液流技术适用于计算植物的臭氧吸收量。  相似文献   

13.
Because of its high resistivity and subsequent low electroactivity, sulfur is not normally considered a room-temperature battery cathode. An elemental sulfur cathode has been made with a measured capacity of over 900 ampere.hours per kilogram, more than 90 percent of the theoretical storage capacity of solid sulfur at room temperature, accessed by means of a lightweight, highly conductive, aqueous polysulfide interface through the electrocatalyzed reaction S + H(2)O + 2e(-) --> HS(-) + OH(-). This solid sulfur cathode was first used in a battery with an aluminum anode for an overall discharge reaction 2Al + 3S + 3OH(-) + 3H(2)O --> 2Al(OH)(3) + 3HS(-), giving a cell potential of 1.3 volts. The theoretical specific energy of the aluminum-sulfur battery (based on potassium salts) is 910 watt.hours per kilogram with an experimental specific energy of up to 220 watt.hours per kilogram.  相似文献   

14.
FACE条件下O3浓度增高对小麦产量和籽粒充实的影响   总被引：1，自引：0，他引：1  
 【目的】探讨近地层大气O3浓度增高对小麦生产的影响。【方法】2007—2009年度应用FACE研究平台,以O3自然浓度(A-O3)为对照,设计O3浓度增高50% (E-O3)进行对比试验,采用烟农19、扬麦16、嘉兴002、扬麦15和扬辐麦2号等5个品种为对象,研究大气O3浓度增高50%对不同基因型小麦品种籽粒产量及其构成因素的影响。【结果】O3浓度增高显著降低小麦籽粒产量,降幅为10.10%—34.51%,平均为19.74%,品种、年度间存在显著或极显著差异。O3浓度增高条件下千粒重降低17.88%(10.16%—29.47%);每穗粒数下降3.47%(-1.53%—11.90%),但穗数平均较对照增加0.95%(-14.58%—23.74%),处理、品种和年度间存在显著或极显著差异。O3浓度增高50%使籽粒长、宽、厚和籽粒体积分别减小0—4.16%、7.95%—20.24%、2.66%—11.00%和8.5%—31.5%;皱缩指数增大0.23%—36.66%,籽粒灌浆速率降低,籽粒充实度变化为-21.40%—3.76%,最终导致粒重降低。【结论】FACE条件下O3浓度增高使籽粒灌浆物质来源不足,籽粒库容变小,充实度降低,粒重变小,最终导致小麦籽粒产量下降。  相似文献   

15.
In ionic crystals of the form M(+)X(-), certain covalently bonded anion groups X(-) are particularly associated with instability. The heavier metal cations M(+) enhance this. Very sensitive explosives occur within the extended azide family, where X(-) = CNO(-), N(3)(-), NCO(-), or NCS(-) (an isoelectronic set of unsaturated linear triatomic anions). Another such family are the globular oxyanions X(-) = ClO(2)(-), ClO(3)(-), ClO(4)(-), NO(3)(-), and MnO(4)(-). Mishandling of NH(4)NO(3) or NH(4)ClO(4) has caused major disasters. An irreversible cyclic mechanism is proposed for such decomposition, involving mechanoelectronic band-gap excitation and coalescence of X with X(-). From an intracrystalline ion-molecule collision complex, the singly charged dianion X(2)(-), exothermic reactions proceed with high yield.  相似文献   

16.
Trivalent aluminum ions are important in natural bodies of water, but the structure of their coordination shell is a complex unsolved problem. In strong acid (pH < 3.0), Al(III) exists almost entirely as the octahedral Al(H2O)6(3+) ion, whereas in basic conditions (pH > 7), a tetrahedral Al(OH)(4- structure prevails. In the biochemically and geochemically critical pH range of 4.3 to 7.0, the ion structures are less clear. Other hydrolytic species, such as AlOH(aq)2+, exist and are traditionally assumed to be hexacoordinate. We show, however, that the kinetics of proton and water exchange on aqueous Al(III), coupled with Car-Parrinello simulations, support a five-coordinate Al(H2O)4OH2+ ion as the predominant form of AlOH(aq)2+ under ambient conditions. This result contrasts Al(III) with other trivalent metal aqua ions, for which there is no evidence for stable pentacoordinate hydrolysis products.  相似文献   

17.
Simultaneous global measurements of nitric acid (HNO(3)), water (H(2)O), chlorine monoxide (CIO), and ozone (O(3)) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO(3) was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H(2)O after mid-July. By mid-August, near the time of peak CIO, abundances of gas-phase HNO(3) and H(2)O were extremely low. The concentrations of HNO(3) and H(2)O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO(3) or H(2)O were observed in the 1992-1993 Arctic winter vortex. Although CIO was enhanced over the Arctic as it was over the Antarctic, Arctic O(3) depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone "hole" is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.  相似文献   

18.
The physical and chemical properties of the hydrated alpha-Al(2)O(3) (0001) surface are important for understanding the reactivity of natural and synthetic aluminum-containing oxides. The structure of this surface was determined in the presence of water vapor at 300 kelvin by crystal truncation rod diffraction at a third-generation synchrotron x-ray source. The fully hydrated surface is oxygen terminated, with a 53% contracted double Al layer directly below. The structure is an intermediate between alpha-Al(2)O(3) and gamma-Al(OH)(3), a fully hydroxylated form of alumina. A semiordered oxygen layer about 2.3 angstroms above the terminal oxygen layer is interpreted as adsorbed water. The clean alpha-Al(2)O(3) (0001) surface, in contrast, is Al terminated and significantly relaxed relative to the bulk structure. These differences explain the different reactivities of the clean and hydroxylated surfaces.  相似文献   

19.
The electronic relaxation dynamics of size-selected (H2O)n-/(D2O)n[25 eaq-(s(dagger)) internal conversion lifetime.  相似文献   

20.
Although 248-nanometer radiation falls 0.12 electron volt short of the energy needed to dissociate O(2) large densities of ozone (O(3)) can be produced from unfocused 248-nanometer KrF excimer laser irradiation of pure O(2). The process is initiated in some undefined manner, possibly through weak two-photon O(2) dissociation, which results in a small amount of O(3) being generated. As soon as any O(3) is present, it strongly absorbs the 248-nanometer radiation and dissociates to vibrationally excited ground state O(2) (among other products), with a quantum yield of 0.1 to 0.15. During the laser pulse, a portion of these molecules absorb a photon and dissociate, which results in the production of three oxygen atoms for one O(3) molecule destroyed. Recombination then converts these atoms to O(3), and thus O(3) production in the system is autocatalytic. A deficiency exists in current models of O(3) photochemistry in the upper stratosphere and mesosphere, in that more O(3) iS found than can be explained. A detailed analysis of the system as it applies to the upper atmosphere is not yet possible, but with reasonable assumptions about O(2) vibrational distributions resulting from O(3) photodissociation and about relaxation rates of vibrationally excited O(2) a case can be made for the importance of incuding this mechanism in the models.  相似文献   

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