Emissions of Oxygenated Volatile Organic Compounds from Plants Part II: Emissions of Saturated Aldehydes

Emissions of hexanal, heptanal, octanal, nonanal, and decanal from 6 different plant species were measured in continuously stirred tank reactors when the plants were exposed to ozone. Pathogen- and insect attack on plants also led to these emissions. The emission rates of individual aldehydes were related to each other implying a common mechanism for the emissions of these aldehydes. Furthermore, the emission pattern was similar in all cases indicating a similar emission mechanism for different plant species and different elicitors. Measurements with ozone exposed Scots pine plants (Pinus sylvestris L.) showed that the emission rates were dependent on temperature as well as on the ozone flux into the plants. The diurnal variation of aldehyde emissions from ozone exposed Scots pine were described quite well using a formalism including temperature and ozone flux as variables. Assuming the aldehyde emissions to be general for plants exposed to ozone, the global emissions were estimated to be in the range between 7 and 22 Tg/a. Because these emissions can be induced by other factors than ozone uptake alone this estimate may be a lower limit.Now atNow at     

Emissions of Oxygenated Volatile Organic Compounds from Plants Part I: Emissions from Lipoxygenase Activity

Emissions of oxygenated volatile organic compounds (OVOC) from several plant species were measured in continuously stirred tank reactors (CSTR). High emission pulses of OVOCs were observed when plants were exposed to stress. Absolute emission rates were highly variable ranging up to 10^–13 mol · cm^–2 · s^–1. The temporal shape of these emissions was described by a formalism similar to that of a consecutive reaction of pseudo first order kinetics. The main emitted OVOC was (Z)-3-hexenol together with other C₆-aldehydes and alcohols, suggesting that lipoxygenase activity on linolenic acid was mainly responsible for OVOC production. Various stress factors induced lipoxygenase activity and subsequent emissions of OVOCs. These factors were exposure to high ozone concentrations, pathogen attack, and wounding. The pattern of OVOC emissions from tobacco was similar for different stress applications and the same products of lipoxygenase activity were emitted from all investigated plant species. Our results imply that these emissions occur as general response of the plants to stress. Since plants experience various abiotic or biotic stress factors in the environment, OVOC emissions as a response to stress are likely to be of significant importance for atmospheric chemistry.Now at     

Emission of Biogenic Volatile Organic Compounds: An Overview of Field, Laboratory and Modelling Studies Performed during the `Tropospheric Research Program' (TFS) 1997–2000

The present paper summarises results on the emission of biogenicvolatile organic compounds (BVOC) achieved within the frame of thenational `German Tropospheric Research Programme' (TFS) between 1997 and2000. Field measurements were carried out at the meteorologicalmonitoring station `Hartheimer Wald' located in the vicinity of Freiburg(upper Rhine valley), Germany, within a pine plantation dominated byScots pine (Pinus sylvestris L.). The measured BVOC emissionrates were used to determine the daily and seasonal variation of BVOCemission and its dependence on important meteorological and plantphysiological parameters. In parallel, laboratory experiments usingyoung trees of pine (P. sylvestris), poplar (Populustremula ×P. alba) and pedunculate oak (Quercusrobur L.) were performed, and the influence of abiotic (e.g.,light, temperature, seasonality, flooding) factors on the biosynthesisand emission of BVOC was quantified. Based on these data, emissionalgorithms were evaluated and a process-oriented numerical model for thesimulation of the isoprene emission by plants was developed. Inaddition, newly calculated land use and tree species distributions wereused for the calculation of an actual BVOC emission inventory ofGermany.     

植物挥发性有机物的初步研究

2000年1～6月期间,美国国家大气研究中心(NCAR)和中国科学院大气物理研究所的科学家发展了一套自动的气相色谱系统和分析方法,用于分析大气中的挥发性有机物.此系统性能稳定,重复性好,对美国大气研究中心附近的大气进行了采样分析.作者简单介绍了此自动系统以及采样分析结果.     

Biogenic Volatile Organic Compounds (VOC): An Overview on Emission, Physiology and Ecology

This overview compiles the actual knowledge of the biogenic emissions of some volatile organic compounds (VOCs), i.e., isoprene, terpenes, alkanes, alkenes, alcohols, esters, carbonyls, and acids. We discuss VOC biosynthesis, emission inventories, relations between emission and plant physiology as well as temperature and radiation, and ecophysiological functions. For isoprene and monoterpenes, an extended summary of standard emission factors, with data related to the plant genus and species, is included. The data compilation shows that we have quite a substantial knowledge of the emission of isoprene and monoterpenes, including emission rates, emission regulation, and biosynthesis. The situation is worse in the case of numerous other compounds (other VOCs or OVOCs) being emitted by the biosphere. This is reflected in the insufficient knowledge of emission rates and biological functions. Except for the terpenoids, only a limited number of studies of OVOCs are available; data are summarized for alkanes, alkenes, carbonyls, alcohols, acids, and esters. In addition to closing these gaps of knowledge, one of the major objectives for future VOC research is improving our knowledge of the fate of organic carbon in the atmosphere, ending up in oxidation products and/or as aerosol particles.     

Volatile Organic Compounds in the Po Basin. Part B: Biogenic VOCs

Measurements of volatile organic compounds (VOCs) were performed in the Po Basin, northern Italy in early summer 1998, summer 2002, and autumn 2003. During the three campaigns, trace gases and meteorological parameters were measured at a semi-rural station, around 35 km north of the city center of Milan. Bimodal diurnal cycles of isoprene with highest concentrations in the morning and evening were found and could be explained by the interaction of emissions, chemical reactions, and vertical mixing. The diurnal cycle could be qualitatively reproduced by a three-dimensional Eulerian model. The nighttime decay of isoprene could be attributed mostly to reactions with NO₃, while the decay of the isoprene oxidation products could not be explained with the considered chemical reactions. Methanol reached very high mixing ratios, up to 150 ppb. High concentrations with considerable variability occurred during nights with high relative humidities and low wind speeds. The origin of these nighttime methanol concentrations is most likely local and biogenic but the specific source could not be identified.     

不同类型草地挥发性有机物排放特征的研究

2003年9月,对内蒙古草原不同类型草地挥发性有机物(VOC)的排放、太阳辐射、气象参数等进行观测,结果表明,固定和新的羊草样地、封育样地、不同程度放牧样地异戊二烯、α蒎烯、β蒎烯、柠檬烯、蒈烯的排放均有明显的日变化规律,并与可见光辐射以及温度有较好的一致性.羊草样地、封育样地、过度放牧、适度放牧样地异戊二烯排放的最大值分别为139.5、25.9、132.3、107.1(单位:μg·m-2·h-1,以碳计).多数情况下,异戊二烯排放通量的测定结果为羊草样地高于封育样地、过度放牧样地高于适度放牧样地.不同程度放牧样地α蒎烯、β蒎烯、柠檬烯、蒈烯等的排放具有明显差别,一般是过度放牧草地高于适度放牧草地.剪草增大了绝大部分VOC组分的排放、以及过度和适度放牧草地VOC的排放,剪草可以造成过度和适度放牧草地异戊二烯排放在中午前后的增加.剪草后,过度放牧草地异戊二烯、α蒎烯、β蒎烯、柠檬烯、蒈烯等的排放通量均远大于适度放牧草地的相应值.土壤异戊二烯、α蒎烯、β蒎烯等的排放很小,分别占相近可见光辐射和温度条件下固定羊草样地排放的0.2%、0、3.0%.     

Air-Sea Exchange of Volatile Organic Compounds: A New Model with Microlayer Effects

The authors propose a new “three-layer” conceptual model for the air-sea exchange of organic gases, which includes a dynamic surface microlayer with photochemical and biological processes. A parameterization of this three-layer model is presented, which was used to calculate the air-sea fluxes of acetone over the Pacific Ocean. The air-sea fluxes of acetone calculated by the three-layer model are in the same direction but possess half the magnitude of the fluxes calculated by the traditional two-layer model in the absence of photochemical and biological processes. However, photochemical and biological processes impacting acetone in the microlayer can greatly vary the calculated fluxes in the three-layer model, even reversing their direction under favorable conditions. Our model may help explain the discrepancies between measured and calculated acetone fluxes in previous studies. More measurements are needed to validate our conceptual model and provide constraints on the model parameters.     

Exchange of Short-Chain Oxygenated Volatile Organic Compounds (VOCs) between Plants and the Atmosphere: A Compilation of Field and Laboratory Studies

Field and laboratory investigations of the exchange of the short-chain organic acids – formic acid and acetic acid – as well as their homologous aldehydes are discussed. Both acids are substantially released from several plant species. Emission measurements under field conditions are compiled to give an overview of three years of measurements. Emission rates from several tree species were found in the range between zero and 60 nmoles m^–2 min^–1 for acetic acid and between zero and 90 nmoles m^–2 min^–1 for formic acid though also a deposition has been observed to orange trees. Investigations under laboratory conditions showed an order of magnitude lower emission rates with significant differences under light and dark conditions, and a deposition was observed under certain conditions. Hence, low emission rates or even a bi-directional exchange, emission as well as deposition have to be taken into account. Further differences between field and laboratory studies are discussed considering age of trees, stress effects and a potential production of acids by photochemical conversion of precursors inside enclosures during sampling. Field data on the exchange of form- and acetaldehyde show a complex behavior. We found emission as well as uptake. The bi-directional exchange is significantly triggered by the ambient mixing ratios of both aldehyde species and exhibits a compensation point. Further studies are needed for generalization of the exchange of these and potentially also for other compounds.     

Gas Chromatographic Determination of Extractable Compounds Composition and Emission Rate of Volatile Terpenes from Larch Needle Litter

A combination of solid-phase microextraction (SPME) and gas chromatography can be successfully used both for establishing the qualitative composition of volatile organic compounds (VOC) emitted by leaf litter and for determining their emission rates. Taking as an example European larch litter, it is shown that dead plant material contains considerable amounts of volatile components as well as non-volatile compounds that can be VOC precursors formed as a result of enzymatic reactions. It is proposed to include the determination of extractable compounds into the methodology of studying litter as a source of atmospheric VOC. Some data on litter mass are reported and it is concluded that this data may be included into special models for emission evaluation. In this work the distribution coefficients of monoterpene hydrocarbons between the gas phase and polydimethylsiloxane fiber coating necessary for quantitative determinations in SPME were estimated.     

Stable Carbon Isotope Ratios and the Photochemical Age of Atmospheric Volatile Organic Compounds

Abstract

The dependence of ozone formation on the mixing ratios of volatile organic compounds (VOCs) and nitrogen oxides (NO_x) has been widely studied. In addition to the atmospheric levels of VOCs and NO_x, the extent of photochemical processing of VOCs has a strong impact on ozone levels. Although methods for measuring atmospheric mixing ratios of VOCs and NO_x are well established and results of those measurements are widely available, determination of the extent of photochemical processing of VOCs, known as photochemical age (PCA), is difficult. In this article a recently developed methodology for the determination of PCA for individual compounds based on the change in their stable carbon isotope composition is used to investigate the dependence between ozone and VOC or NO_x mixing ratios at a rural site in Ontario, Canada, during fall and winter. The results show that under these conditions the variability in VOC mixing ratios is predominantly a result of the varying impact of local emissions and not a result of changes in the extent of atmospheric processing. This explains why the mixing ratio of ozone shows no systematic dependence on the mixing ratios of VOCs or NO_x in this environment and at this time of the year.     

复播油葵栽培方式及小气候特征试验研究

通过复播油葵不同栽培方式及小气候特征的试验研究，得出起垄沟播较对照发育期进程、生长量、地温、节水均效果显著。     

Comparability of Biogenic VOC Emission Rate Measurements under Laboratory and Ambient Conditions at the Example of Monoterpene Emissions from Scots Pine (Pinus sylvestris)

Laboratory experiments under controlled environmental conditions are a useful tool to investigate the influence of different environmental parameters on VOC emissions from plants individually. Before using the obtained results to interpret measurements under ambient conditions, it has to be ensured that the laboratory system is suitable for performing emission rate measurements under ambient-like conditions to derive algorithms describing the emissions of volatile organic compounds as a function of physical variables like temperature and light intensity. Here we compare results from monoterpene emission rate measurements with Scots pines (Pinus sylvestris L.) under both ambient environmental conditions using a mobile plant enclosure chamber, and under controlled laboratory conditions in a continuously stirred tank reactor. The different analytical instruments to quantify monoterpene emissions were compared in an intercalibration experiment. Measurements of the mixing ratios of -pinene, -pinene, 3-carene, camphene, and limonene on the order of some hundred parts per trillion differed by less than 20%. The laboratory system has proven capable of providing ambient-like conditions and results of monoterpene emission rate measurements under laboratory conditions could be extrapolated to the natural environment. Monoterpene emission rate measurements with identical specimens of Scots pines conducted within small temporal differences under similar laboratory and outdoor conditions agreed well. Both laboratory and outdoor experiments clearly showed that distinct and constant values neither exist for the standard emission rates nor for the emission pattern of monoterpenes from Scots pine. Temporal variations in the standard emission rates from identical specimens and plant-to-plant variations were on the order of one magnitude.     

基于排放源的中国城市垃圾填埋场甲烷排放研究

利用全国垃圾填埋场的点源数据,基于实际调研和实验室分析建立中国不同区域、不同规模、不同填埋时间的排放因子矩阵,采用IPCC推荐的一级降解动力学（FOD）方法自下而上地核算了中国2107个垃圾填埋场在2007年的甲烷（CH₄）排放量。针对不同区域和类型的填埋场,分别就城市垃圾组分、可降解有机碳、CH₄修正因子、CH₄氧化系数、填埋场CH₄收集率等进行了深入研究。结果显示,中国2007年填埋场CH₄排放量为118.61万t,与《中华人民共和国气候变化第二次国家信息通报》2005年填埋场排放量（220万t）差异较大,其主要原因是城市垃圾填埋场统计数据的差异,例如填埋场个数及垃圾填埋量。中国绝大部分填埋场CH₄年排放量在700 t以下,超过1000 t的有279个,超过1万t的仅10个。江苏省的CH₄排放量最高,达到9.87万t;西藏的排放量最小,仅为0.21万t。东部江苏、广东、浙江等省的整体排放量较高,西部地区西藏、宁夏、青海等地的排放水平较低。     

海南岛和厦门红树林湿地CH4 排放的时空变化

研究了海南岛和厦门的河口海岸红树林湿地、海岸光滩及红树林伐迹地CH4排放的时空变化。海南岛长宁站位海莲林连续两年的CH4排放率均表现为外滩>中滩>内滩的空间变化模式,与土壤含水量的空间变化一致,而与土壤盐度的空间变化相反;但1997年在其余五个红树林湿地的CH4排放率表现出不同的空间变化规律,且大多与土壤理化因子不呈对应关系。各红树林湿地的最低CH4排放率均出现在冬季。红树林湿地年CH4排放率高于海岸光滩而低于红树林伐迹地。     

Vertical Evolution of Boundary Layer Volatile Organic Compounds in Summer over the North China Plain and the Differences with Winter

The vertical observation of volatile organic compounds(VOCs) is an important means to clarify the mechanisms of ozone formation. To explore the vertical evolution of VOCs in summer, a field campaign using a tethered balloon during summer photochemical pollution was conducted in Shijiazhuang from 8 June to 3 July 2019. A total of 192 samples were collected, 23 vertical profiles were obtained, and the concentrations of 87 VOCs were measured. The range of the total VOC concentration was 41–48 ppbv below 600 m. It then slightly increased above 600 m, and rose to 58 ± 52 ppbv at 1000 m.The proportion of alkanes increased with height, while the proportions of alkenes, halohydrocarbons and acetylene decreased. The proportion of aromatics remained almost unchanged. A comparison with the results of a winter field campaign during 8–16 January 2019 showed that the concentrations of all VOCs in winter except for halohydrocarbons were more than twice those in summer. Alkanes accounted for the same proportion in winter and summer. Alkenes,aromatics, and acetylene accounted for higher proportions in winter, while halohydrocarbons accounted for a higher proportion in summer. There were five VOC sources in the vertical direction. The proportions of gasoline vehicular emissions + industrial sources and coal burning were higher in winter. The proportions of biogenic sources + long-range transport, solvent usage, and diesel vehicular emissions were higher in summer. From the surface to 1000 m, the proportion of gasoline vehicular emissions + industrial sources gradually increased.     

Profiles and Source Apportionment of Nonmethane Volatile Organic Compounds in Winter and Summer in Xi’an,China, based on the Hybrid Environmental Receptor Model

Summer and winter campaigns for the chemical compositions and sources of nonmethane hydrocarbons(NMHCs)and oxygenated volatile organic compounds(OVOCs)were conducted in Xi’an.Data from 57 photochemical assessment monitoring stations for NMHCs and 20 OVOC species were analyzed.Significant seasonal differences were noted for total VOC(TVOC,NMHCs and OVOCs)concentrations and compositions.The campaign-average TVOC concentrations in winter(85.3±60.6 ppbv)were almost twice those in summer(47.2±31.6 ppbv).Alkanes and OVOCs were the most abundant category in winter and summer,respectively.NMHCs,but not OVOCs,had significantly higher levels on weekends than on weekdays.Total ozone formation potential was higher in summer than in winter(by 50%)because of the high concentrations of alkenes(particularly isoprene),high temperature,and high solar radiation levels in summer.The Hybrid Environmental Receptor Model(HERM)was used to conduct source apportionment for atmospheric TVOCs in winter and summer,with excellent accuracy.HERM demonstrated its suitability in a situation where only partial source profile data were available.The HERM results indicated significantly different seasonal source contributions to TVOCs in Xi’an.In particular,coal and biomass burning had contributions greater than half in winter(53.4%),whereas traffic sources were prevalent in summer(53.1%).This study’s results highlight the need for targeted and adjustable VOC control measures that account for seasonal differences in Xi’an;such measures should target not only the severe problem with VOC pollution but also the problem of consequent secondary pollution(e.g.,from ozone and secondary organic aerosols).     

Estimates of monoterpene and isoprene emissions from the forests in Switzerland

Emission rates of biogenic volatile organic compounds emitted by the forests were estimated for five geographical regions as well as for all Switzerland. Monoterpene and isoprene emissions rates were calculated for each main tree species separately using the relevant parameters such as temperature, light intensity and leaf biomass density. Biogenic emissions from the forests were found to be about 23% of the total annual VOC emissions (anthropogenic and biogenic) in Switzerland. The highest emissions are in July and lowest in January. Calculations showed that the coniferous trees are the main sources of the biogenic emissions. The major contribution comes from the Norway spruce (picea abies) forests due to their abundance and high leaf biomass density. Although broad-leaved forests cover 27% of all the forests in Switzerland, their contribution to the biogenic emissions is only 3%. Monoterpenes are the main species emitted, whereas only 3% is released as isoprene. The highest emission rates of biogenic VOC are estimated to be in the region of the Alps which has the largest forest coverage in Switzerland and the major part of these forests consists of Norway spruce. The total annual biogenic VOC emission rate of 87 ktonnes y^–1 coming from the forests is significantly higher than those from other studies where calculations were carried out by classifying the forests as deciduous and coniferous. The difference is attributed to the high leaf biomass densities of Norway spruce and fir (abies alba) trees which have a strong effect on the results when speciation of trees is taken into account. Besides the annual rate, emission rates were calculated for a specific period during July 4–6, 1991 when a photochemical smog episode was investigated in the Swiss field experiment POLLUMET. Emission rates estimated for that period agree well with those calculated for July using the average temperatures over the last 10 years.     

The impact of the Tokyo Metropolitan Emissions Trading Scheme on reducing greenhouse gas emissions: findings from a facility-based study

This paper provides a detailed analysis of the Tokyo Metropolitan Emissions Trading Scheme (Tokyo ETS), Japan’s first emissions trading scheme with mandatory cap initiated by the government of Tokyo. Unlike trading schemes in other countries, the Tokyo ETS covers indirect emissions from the commercial sector. It is well known that a variety of market barriers impede full realization of energy efficiency opportunities, especially in the commercial sector. Experiences with the Tokyo ETS should therefore provide important lessons for the design of climate change mitigation policies, especially when targeting the commercial sector. The emissions from covered entities have been drastically reduced from those at the scheme’s outset, with an average 14% reduction as of the end of the first commitment period of five years (2010–2014) compared with 2009 levels. This paper shows that the Tokyo ETS alone did not cause these reductions; there were other drivers. Among them, the energy savings triggered by the Great East Japan Earthquake in 2011 were crucial. The contribution of credit trading, in contrast, was limited since most of the covered entities reduced emissions by themselves. Through an investigation of official reports, an assessment of the emissions data from the covered entities compared to those of uncovered entities and in-depth interviews with firms covered by the scheme, this paper confirms that the main drivers of emissions reductions by covered entities were separate from the ETS. In fact, the advisory aspect of the scheme seems to be much more important in encouraging energy-saving actions.

Key policy insights

• Most of the observed emission reductions were not caused by the Tokyo ETS alone.

• An advisory instrument was crucial to the effectiveness of the Tokyo ETS.

• The experience of the Tokyo ETS suggests that making full use of the advantages of emissions trading is difficult in the case of the commercial sector.

• Price signals have not provided a stimulus to climate change mitigation actions, which implies that establishing a cap to yield effective carbon prices poses a challenge.

     

月尺度气温可预报性对资料长度的依赖及可信度

利用全国518个站1960—2011年逐日气温观测资料和160个站1983—2012年月尺度气温客观预测数据,基于非线性局部Lyapunov指数和非线性误差增长理论,研究中国区域月尺度气温可预报性期限对资料序列长度的依赖性。结果表明:气温可预报性期限对资料序列的长度有一定程度的依赖性,在西北、东北及华中地区尤为明显。平均而言,45年的资料序列长度才能够得到稳定合理的可预报性期限。为了验证气温可预报期限计算结果的可信度,将月尺度气温的可预报性期限与客观气候预测方法的预报评分技巧进行对比,发现两者结果非常一致。其中,由观测资料得到的1月气温的可预报性期限明显低于7月,1月客观气候预测方法的预报评分技巧也明显低于7月,且1月 (7月) 预报评分的空间分布型与1月 (7月) 气温可预报性期限的空间分布型较为一致。因此,利用非线性局部Lyapunov指数和台站逐日观测资料分析气温的可预报性期限结果是可信的。