海岸带盐沼生态系统卤代甲烷释放研究进展

卤代甲烷是破坏臭氧层的主要物质,也是重要的痕量温室气体和有机污染物.目前,其源汇格局和全球收支存在很大的不确定性.受海陆两相交互作用影响的海岸带盐沼是卤代甲烷重要的自然来源.本文综述了卤代甲烷自然源汇的研究现状、海岸带盐沼卤代甲烷的释放规律以及主要影响因素.鉴于当前研究中存在的问题,其后的研究需在以下几个方面进一步加强: 1)较长时间尺度、更大区域范围的盐沼卤代甲烷释放规律及源汇评估研究;2)利用目前已比较成熟的稳定同位素技术,更精确地定量不同盐生植物种类以及各种生物类型对盐沼卤代甲烷的贡献比率;3)关注潮水对其产生的直接或间接影响,进一步研究潮汐涨落过程、淹水时长等对盐沼卤代甲烷释放的影响;4)人类活动和气候变化对盐沼卤代甲烷释放的影响.     

陆地生态系统碳源与碳汇及其影响机制研究进展

全球碳循环研究中发现,目前已知碳源与碳汇不能达到平衡。存在一个很大的碳失汇。大气、海洋和陆地生态系统是人工源CO2的3个可能的容纳汇,其中陆地生态系统最复杂、最具不确定性,因此陆地生态系统碳源与碳汇研究是全球碳循环研究的核心问题之一。大气成分监测、CO2通量测定、森林资源清查以及模型模拟等方面的研究都表明,CO2施肥效应、氮沉降增加、污染、全球气候变化以及土地利用变化,是影响陆地生态系统碳储量的主要生态机制,但不确定在过去的10～100年以及未来哪一种机制起最主要的作用。     

冻土甲烷循环微生物群落及其对全球变化的响应

冻土是陆地生态系统中最容易受到全球气候变化影响的碳库,既发挥着碳源又起着碳汇的作用。人们非常关注贮存于冻土中有机碳的最终归宿,是因为全球气候变暖会加快冻土的解冻,释放更多的温室气体（二氧化碳和甲烷）到大气中,从而进一步加剧温室效应。据估计每年从北半球冻原陆地生态系统释放进入大气的甲烷约占全球自然界释放甲烷总量的25%。研究证实冻土生物源甲烷的产生和消耗分别由耐(嗜)低温的产甲烷菌(methanogens)和甲烷氧化菌(methanotrophs)介导。鉴于冻土甲烷循环对全球甲烷平衡的显著作用以及在冻土生物地球化学循环中的重要功能,对介导冻土甲烷循环的产甲烷菌和甲烷氧化菌的研究将有助于更好地评估冻土生态系统对全球气候变化的响应和影响,本文就冻土甲烷循环过程、产甲烷菌、甲烷氧化菌的群落结构、活动、生态功能及其对气候和环境变化的响应机制的最新研究进行综述,以期为我国开展冻土甲烷循环机理研究提供支持。     

大气甲烷的源和汇与土壤氧化 (吸收)甲烷研究进展

甲烷是主要的温室气体之一,对温室效应的贡献仅次于CO₂,而每分子甲烷温室增温潜力是CO₂的21倍.因此确定全球大气甲烷的源与汇,并对其进行估算、预测已成为目前全球环境变化及温室效应研究的一个热点.本文概述了国内外大气甲烷源与汇研究的进展情况,详述了土壤氧化(吸收)大气与内源甲烷机理及其影响因子(如土地利用情况、环境甲烷浓度、土壤温度、湿度、pH值、孔隙状况等).最后指出,通过在长白山森林垂直分布带开展地带性土壤甲烷氧化(吸收)研究,对估算我国温带至寒带、高山苔原带土壤吸收甲烷总量,乃至全球甲烷汇具有重要意义.     

垃圾填埋场甲烷氧化菌及甲烷减排的研究进展

垃圾填埋场是全球最重要的人为甲烷排放源之一,其全球年甲烷释放量为35-69 Tg,垃圾填埋场甲烷减排是目前全球温室气体研究的热点。甲烷氧化菌能够氧化分解甲烷,作为减少大气甲烷排放的重要生物汇,对保持大气中甲烷浓度的平衡具有重要意义。从甲烷氧化菌的类型及其特征、甲烷氧化机理着手,介绍了多样性研究方法、填埋场中甲烷氧化菌的活性影响因素及甲烷生物减排应用等最新研究进展。在综述前人研究的基础上,探讨了目前研究的不足,提出了利用甲烷氧化菌复合微生物菌剂等综合处理措施,旨为垃圾填埋场甲烷减排的研究和应用提供新的思路。     

大气二氧化碳浓度增加对木本植物BVOCs释放的影响

植物挥发性有机化合物(biogenic volatile organic compounds,BVOCs)在近地表臭氧和二次有机气溶胶生成中有重要作用,而大气CO2浓度上升对植物BVOCs释放有显著影响。利用Meta-analysis方法对已发表的数据进行整合分析发现:(1)总体而言,大气CO2浓度增加会导致不同木本植物(常绿与落叶)BVOCs释放降低;(2)就不同木本植物BVOCs释放而言,大气CO2浓度增加主要导致落叶植物BVOCs释放速率降低,而常绿植物则以增加为主;(3)就植物释放BVOCs种类而言,大气CO2浓度增加显著降低异戊二烯的释放速率,对单萜烯释放速率则无显著影响。结果可为阐明陆地生态系统BVOCs释放对全球CO2浓度增加的响应提供依据。     

大气甲烷的源和汇与土壤氧化(吸收)甲烷研究进展

甲烷是主要的温室气体之一,对温室效应的贡献仅次于CO2,而每分子甲烷温室增温潜力是CO2的21倍,因此确定全球大气甲烷的源与汇,并与其进行估算,预测已成为目前全球环境变化及温室效应研究的一个热点。本文概述了国内外大气甲烷烷源与汇研究的进展情况,详述了土壤氧化（吸收）大气与内源甲烷机理及其影响因子（如土地利用情况,环境甲烷浓度,土壤温度,湿度,pH值,孔隙状况等）,最后指出,通过在长白山森林垂直分布带开展地带性土壤甲烷氧化（吸收）研究,对估算我国温带至寒带,高山苔原带土壤吸收甲烷含量,乃至全球甲烷汇具有重要意义。     

中国陆地生态系统碳源/汇整合分析

国家尺度陆地生态系统碳收支及其循环过程的研究对于提升地球系统科学与全球变化科学的科技创新能力、提高我国参与应对全球气候变化国际行动和维护国家利益的话语权、保障国家生态安全和改进生态系统管理都具有重要意义。近年来,我国已经在气候变化与陆地生态系统碳循环领域开展了大量的研究工作,主要包括国家清查、生态系统模型模拟、大气反演等手段。然而,由于大尺度陆地生态系统碳源/汇的估算存在很大的不确定性,目前尚未形成国家尺度的陆地生态系统碳源/汇的整合分析。通过搜集已发表的关于中国陆地生态系统及其组分碳源/汇的59篇文献,整合国家清查、生态系统模型模拟、大气反演3种研究手段,分析中国陆地生态系统碳源/汇大小以及时间尺度上的动态变化。结果表明,在1960s-2010s期间中国陆地生态系统碳汇整体呈上升趋势,平均为（0.213±0.030）Pg C/a,其中森林、草地、农田和灌木生态系统碳汇分别为（0.101±0.023）Pg C/a、（0.032±0.007）Pg C/a、（0.043±0.010）Pg C/a和（0.028±0.010）Pg C/a。森林生态系统中的植被碳汇远大于土壤碳汇,然而这种格局在草地和农田生态系统却相反,而且1960s-2010s期间中国主要植被类型的生态系统碳汇总体上随时间呈增加趋势。融合多源数据（地面观测、激光雷达、卫星遥感等）、多尺度数据（样地尺度、站点尺度、区域尺度）以及多手段数据（联网观测、森林清查、模型模拟）,有助于全面准确地评估中国陆地生态系统碳源/汇及其对气候变化的响应。     

增氮对青藏高原东缘高寒草甸土壤甲烷吸收的早期影响

研究大气氮沉降对青藏高原高寒草甸土壤CH4吸收的影响,对于揭示氮素调节土壤CH4吸收的机制和评价氮沉降增加背景下大气CH4收支平衡至关重要.通过构建多形态、低剂量的增氮控制试验,测定土壤CH4净交换通量和相关土壤理化性质,分析高寒草甸土壤CH4通量变化特征及其主要驱动因子.研究结果表明:自然状态下高寒草甸土壤是大气CH4汇,CH4平均吸收量为(35.40±1.92) μg· m-2· h-1.土壤CH4吸收主要受水分驱动,其次为土壤NH4+-N和NO3-N含量.NH4+-N抑制CH4吸收,NO3--N促进CH4吸收;不同剂量氮素输入对土壤CH4吸收影响也不尽相同,低氮处理促进土壤CH4吸收,而中氮和高氮处理抑制土壤CH4吸收.结果显示青藏高原高寒草甸土壤是重要的大气CH4汇,在未来大气氮沉降加倍的情景下CH4汇功能增强,但当氮沉降量增加两倍以上时CH4汇功能将会减弱.     

大气CO2增加对陆地生态系统微量气体地-气交换的影响

简要综述了近年来国内外在大气CO2浓度增加对微量气体交换影响方面的研究进展,首先介绍了有关大气CO2浓度增加的研究技术和方法,比较了目前两种常用技术开顶箱（OTC）和开放式空气CO2增加（FACE）方法的优缺点,然后着重阐述了用OTC和FACE研究陆地生态系统CH4、N2O、CO2等微量气体的地气交换对大气CO2浓度增加的响应,综合现有的资料表明,大气CO2浓度增加,会促进绿色植物生物量增加,同时改变生物质的C/N,降低有机质的分解速率,增强了陆地生态系统对大气CO2的固特作用;大气CO2浓度增加会提高产甲烷菌的活性和影响CH4的排放过程,有可能导致湿地生态系统CH4的排放增加;大气CO2浓度增加对N2O排放影响的研究较少,且尚无一致的结论;另外,对于其他微量气体,尚没有盯关研究报道,鉴于此,今后应加强大气CO2浓度增加的微量气体地气交换响应研究。     

Genetic control of methyl halide production in Arabidopsis

Methyl chloride (CH(3)Cl) and methyl bromide (CH(3)Br) are the primary carriers of natural chlorine and bromine, respectively, to the stratosphere, where they catalyze the destruction of ozone, whereas methyl iodide (CH(3)I) influences aerosol formation and ozone loss in the boundary layer. CH(3)Br is also an agricultural pesticide whose use is regulated by international agreement. Despite the economic and environmental importance of these methyl halides, their natural sources and biological production mechanisms are poorly understood. Besides CH(3)Br fumigation, important sources include oceans, biomass burning, tropical plants, salt marshes, and certain crops and fungi. Here, we demonstrate that the model plant Arabidopsis thaliana produces and emits methyl halides and that the enzyme primarily responsible for the production is encoded by the HARMLESS TO OZONE LAYER (HOL) gene. The encoded protein belongs to a group of methyltransferases capable of catalyzing the S-adenosyl-L-methionine (SAM)-dependent methylation of chloride (Cl(-)), bromide (Br(-)), and iodide (I(-)) to produce methyl halides. In mutant plants with the HOL gene disrupted, methyl halide production is largely eliminated. A phylogenetic analysis with the HOL gene suggests that the ability to produce methyl halides is widespread among vascular plants. This approach provides a genetic basis for understanding and predicting patterns of methyl halide production by plants.     

Description of toluene inhibition of methyl bromide biodegradation in seawater and isolation of a marine toluene oxidizer that degrades methyl bromide

Methyl bromide (CH3Br) and methyl chloride (CH3Cl) are important precursors for destruction of stratospheric ozone, and oceanic uptake is an important component of the biogeochemical cycle of these methyl halides. In an effort to identify and characterize the organisms mediating halocarbon biodegradation, we surveyed the effect of potential cometabolic substrates on CH3Br biodegradation using a 13CH3Br incubation technique. Toluene (160 to 200 nM) clearly inhibited CH3Br and CH3Cl degradation in seawater samples from the North Atlantic, North Pacific, and Southern Oceans. Furthermore, a marine bacterium able to co-oxidize CH3Br while growing on toluene was isolated from subtropical Western Atlantic seawater. The bacterium, Oxy6, was also able to oxidize o-xylene and the xylene monooxygenase (XMO) pathway intermediate 3-methylcatechol. Patterns of substrate oxidation, lack of acetylene inhibition, and the inability of the toluene 4-monooxygenase (T4MO)-containing bacterium Pseudomonas mendocina KR1 to degrade CH3Br ruled out participation of the T4MO pathway in Oxy6. Oxy6 also oxidized a variety of toluene (TOL) pathway intermediates such as benzyl alcohol, benzylaldehyde, benzoate, and catechol, but the inability of Pseudomonas putida mt-2 to degrade CH3Br suggested that the TOL pathway might not be responsible for CH3Br biodegradation. Molecular phylogenetic analysis identified Oxy6 to be a member of the family Sphingomonadaceae related to species within the Porphyrobacter genus. Although some Sphingomonadaceae can degrade a variety of xenobiotic compounds, this appears to be the first report of CH3Br degradation for this class of organism. The widespread inhibitory effect of toluene on natural seawater samples and the metabolic capabilities of Oxy6 indicate a possible link between aromatic hydrocarbon utilization and the biogeochemical cycle of methyl halides.     

Fluorescence-Based Bacterial Bioreporter for Specific Detection of Methyl Halide Emissions in the Environment

Methyl halides are volatile one-carbon compounds responsible for substantial depletion of stratospheric ozone. Among them, chloromethane (CH₃Cl) is the most abundant halogenated hydrocarbon in the atmosphere. Global budgets of methyl halides in the environment are still poorly understood due to uncertainties in their natural sources, mainly from vegetation, and their sinks, which include chloromethane-degrading bacteria. A bacterial bioreporter for the detection of methyl halides was developed on the basis of detailed knowledge of the physiology and genetics of Methylobacterium extorquens CM4, an aerobic alphaproteobacterium which utilizes chloromethane as the sole source of carbon and energy. A plasmid construct with the promoter region of the chloromethane dehalogenase gene cmuA fused to a promotorless yellow fluorescent protein gene cassette resulted in specific methyl halide-dependent fluorescence when introduced into M. extorquens CM4. The bacterial whole-cell bioreporter allowed detection of methyl halides at femtomolar levels and quantification at concentrations above 10 pM (approximately 240 ppt). As shown for the model chloromethane-producing plant Arabidopsis thaliana in particular, the bioreporter may provide an attractive alternative to analytical chemical methods to screen for natural sources of methyl halide emissions.     

Bacteria mediate methylation of iodine in marine and terrestrial environments

Methyl iodide (CH(3)I) plays an important role in the natural iodine cycle and participates in atmospheric ozone destruction. However, the main source of this compound in nature is still unclear. Here we report that a wide variety of bacteria including terrestrial and marine bacteria are capable of methylating the environmental level of iodide (0.1 microM). Of the strains tested, Rhizobium sp. strain MRCD 19 was chosen for further analysis, and it was found that the cell extract catalyzed the methylation of iodide with S-adenosyl-L-methionine as the methyl donor. These results strongly indicate that bacteria contribute to iodine transfer from the terrestrial and marine ecosystems into the atmosphere.     

Isolation and characterization of a gene encoding a S-adenosyl-l-methionine-dependent halide/thiol methyltransferase (HTMT) from the marine diatom Phaeodactylum tricornutum: Biogenic mechanism of CH(3)I emissions in oceans

Several marine algae including diatoms exhibit S-adenosyl-l-methionine (SAM) halide/thiol methyltransferase (HTMT) activity, which is involved in the emission of methyl halides. In this study, the in vivo biogenic emission of methyl iodide from the diatom Phaeodactylum tricornutum was found to be clearly correlated with iodide concentration in the incubation media. The gene encoding HTMT (Pthtmt) was isolated from P. tricornutum CCAP 1055/1, and expressed in Escherichia coli. The molecular weight of the enzyme was 29.7kDa including a histidine tag, and the optimal pH was around pH 7.0. The kinetic properties of recombinant PtHTMT towards Cl(-), Br(-), I(-), [SH](-), [SCN](-), and SAM were 637.88mM, 72.83mM, 8.60mM, 9.92mM, 7.9mM, and 0.016mM, respectively, and were similar to those of higher-plant HTMTs, except that the activity towards thiocyanate was lower. The biogenic emission of methyl halides from the cultured cells and the enzymatic properties of HTMT suggest that the HMT/HTMT reaction is key to understanding the biogenesis of methyl halides in oceanic environments as well as terrestrial ones.     

大气溴甲烷的释放与控制研究

大气溴甲烷是破坏大气臭氧层的主要化合物之一,既有人为释放,也有自然释放,目前还存在着巨大的未知源。了解大气溴甲烷释放规律和控制措施,不仅对保护臭氧层具有重要意义,而且是大气溴甲烷含量的历史追溯和未来预测的重要基础,是全球变化研究热点。全面介绍了大气溴甲烷排放的途径和机制以及调控排放通量的主要措施,并分析了近期的优先研究领域。     

Ectomycorrhizal fungi: A new source of atmospheric methyl halides?

Incomplete source budgets for methyl halides – compounds that release inorganic chlorine and bromine radicals which, in turn, catalyze atmospheric ozone depletion – limit our ability to predict the fate of the stratospheric ozone layer. We report here the first measured emissions of methyl chloride, methyl bromide, and methyl iodide from ectomycorrhizal fungi. We grew nine fungal isolates on growth media containing halide concentrations similar to those found in soils and plant tissues. The observed range of emissions was 0.003–65 μg methyl chloride, 0.001–3 μg methyl bromide, and 0.02–12 μg methyl iodide g^?1 dry weight fungi day^?1. Species varied in production rates of methyl chloride vs. methyl bromide vs. methyl iodide. Cenococcum geophilum, a widespread ectomycorrhizal fungus, was further tested to investigate the effects of halide substrate concentration in growth media. Emissions from this species increased linearly with increasing concentrations of both bromide and iodide. In addition, a subset of four fungi was studied with two media concentrations each of chloride, bromide, and iodide (0.2 or 20 mm ). These fungi had similar responses to halide concentration, despite 1000‐fold differences in baseline emission rates between isolates. Finally, high chloride concentrations (20 mm ) in media did not appear to inhibit emissions of methyl bromide or methyl iodide. Overall, ectomycorrhizal fungi might be an important source of methyl halides to the atmosphere, and substrate concentrations and community composition may influence production levels in ecosystems.     

Involvement of S-adenosylmethionine-dependent halide/thiol methyltransferase (HTMT) in methyl halide emissions from agricultural plants: isolation and characterization of an HTMT-coding gene from Raphanus sativus (daikon radish)

Background  

Biogenic emissions of methyl halides (CH₃Cl, CH₃Br and CH₃I) are the major source of these compounds in the atmosphere; however, there are few reports about the halide profiles and strengths of these emissions. Halide ion methyltransferase (HMT) and halide/thiol methyltransferase (HTMT) enzymes concerning these emissions have been purified and characterized from several organisms including marine algae, fungi, and higher plants; however, the correlation between emission profiles of methyl halides and the enzymatic properties of HMT/HTMT, and their role in vivo remains unclear.     

Theoretical studies on identity SN2 reactions of lithium halide and methyl halide: A microhydration model

Reactions of lithium halide (LiX, X = F, Cl, Br and I) and methyl halide (CH₃X, X = F, Cl, Br and I) have been investigated at the B3LYP/6-31G(d) level of theory using the microhydration model. Beginning with hydrated lithium ion, four or two water molecules have been conveniently introduced to these aqueous-phase halogen-exchange S_N2 reactions. These water molecules coordinated with the center metal lithium ion, and also interacted with entering and leaving halogen anion via hydrogen bond in complexes and transition state, which to some extent compensated hydration of halogen anion. At 298 K the reaction profiles all involve central barriers ΔE _cent which are found to decrease in the order F > Cl > Br > I. The same trend is also found for the overall barriers (ΔE _ovr ) of the title reaction. In the S_N2 reaction of sodium iodide and methyl iodide, the activation energy agrees well with the aqueous conductometric investigation.