工厂化堆肥温室气体排放和氨气同位素特征

畜禽废弃物堆肥处理过程中产生的二氧化碳(CO₂)、氧化亚氮(N₂O)、甲烷(CH₄)和氨气(NH₃)等是重要的温室气体和大气污染物。但目前有关该过程气体排放的研究多基于室内小型模拟的反应器式堆肥,在工厂化堆肥条件下的原位气体排放监测较少。为探究工厂化堆肥产生气体对区域环境的影响,本研究对沈阳某堆肥厂畜禽废弃物堆体的气体排放进行了19 d的监测,并量化了排放氨气的自然丰度¹⁵N(δ¹⁵N)特征。结果表明: 堆置周期内,CO₂、CH₄、N₂O和NH₃的平均排放速率分别为86.8 g CO₂-C·d^-1·m^-2、9.8 g CH₄-C·d^-1·m^-2、3.7 mg N₂O-N·d^-1·m^-2和736.6 mg NH₃-N·d^-1·m^-2。温室气体日增温潜势(GWP)的贡献大小为CH₄>CO₂>NH₃(间接)>N₂O,其中CH₄贡献了65％。堆肥排放NH₃的δ¹⁵N在-21.8‰～-7.2‰,平均-11.6‰±1.2‰。本研究结果可为区域畜禽废弃物堆肥过程中温室气体排放的核算及大气氨溯源提供数据支持。     

开放式空气CO2增高对稻田CH4和N2O排放的影响

在FACE(free-aircarbondioxideenrichment)平台上,采用静态暗箱气相色谱法观测研究了大气CO₂浓度增加对稻田CH₄和N₂O排放的影响.结果表明,在150和250kgN·hm^-2两种氮肥水平下大气CO₂浓度增加200μmol·mol^-1均明显促进水稻生长,水稻生物量积累.大气CO₂浓度增加对150和250kgN·hm^-2两种氮肥水平下稻田CH₄排放均无显著影响,并简要分析了与现有文献报道结果不一致的原因.大气CO₂浓度增加也未导致150和250kgN·hm^-2两种氮肥水平下稻田N₂O排放的明显变化,与大多数研究结果一致.     

日本长期不同施肥稻田N2O和CH4排放特征及其环境影响

观测了75年长期连续不施肥、施硫酸铵、施熟制水稻秸秆与豆饼混合堆肥、施绿肥苜蓿4种处理下日本单季稻田温室气体N₂O和CH₄的排放特征及其环境影响.结果表明： 在水稻生长季节,不同处理间N₂O排放无显著差异,但CH₄排放差异显著;长期连续施用有机肥虽然没有增加N₂O排放却促进了CH₄排放.各系统排放N₂O和CH₄所产生的累积全球增温潜势（GWP）以绿肥处理最大（310.7 g CO₂e·m^-2）,熟制有机堆肥次之（151g CO₂e·m^-2）,硫酸铵处理最小（60.6 g CO₂e·m^-2）.稻田系统的GWP主要来自CH₄排放,控制和减少稻田系统CH₄排放是稻田温室气体减排的核心问题.长期连续施用熟制有机堆肥既能增加土壤有机质,改善地力,满足水稻高产,又能实现CH₄减排,是实践中值得推荐的水稻生产模式.     

稻田CH4和N2O的排放及养萍和施肥的影响

用箱法对我国东北稻田CH₄和N₂O排放进行观测研究表明,东北稻田的CH₄排放通量比南方稻田小,平均日排放通量和生长季节排放总量分别为0.07和7.4g·m^-2.稻田淹水期几乎没有N₂O的净排放,但在非淹水期内却有大量N₂O排放(平均通量59μgN₂O·m^-2·h^-1).稻田养萍和施肥明显促进CH₄和N₂O排放。稻田CH₄和N₂O排放之间存在消长关系。制定稻田温室气体减排技术措施时应充分注意这一关系。     

不同灌溉措施下春玉米田间N2O和CO2日变化特征及影响因素研究

为探究西辽河平原浅埋滴灌下春玉米田N₂O和CO₂排放通量日变化特征及其影响因素,并确定1天中最佳观测时间。在春玉米吐丝期,采用静态暗箱-气相色谱法研究大水漫灌(CK)和浅埋滴灌(DG)处理N₂O和CO₂日排放动态变化特征,并分析其与土壤温度和湿度相关性。结果表明,在浅埋滴灌和大水漫灌两种灌溉方式下N₂O和CO₂排放具有明显的日变化特征,日变化趋势与大气温度变化相似,呈单峰型排放曲线,排放峰值均出现在观测当天大气温度达到最高值后2小时左右。大水漫灌N₂O和CO₂日排放通量均值分别为199.21μg·m^-2·h^-1、217.77 mg·m^-2·h^-1;浅埋滴灌N₂O和CO₂日排放通量均值分别为235.82μg·m^-2·h^-1、253.54 mg...     

广州地区晚稻田 CH4和N2O 的排放通量及其影响因素

用密闭箱法同时研究了广州地区晚稻田CH₄和N₂O的排放通量。结果表明,连续淹水、常规连作和水旱轮作等3种处理的CH₄平均排放通量分别为1.763、2.84和0.36mg·m^-2·h^-1,而N₂O的平均排放通量分别为6.74、11.69和55.07μgN₂O-N·m^-2·h^-1,表明稻田连续淹水显著增加CH₄的排放而降低N₂O的排放。水旱轮作降低CH₄排放而提高N₂O的排放,说明稻田CH₄和N₂O排放之间存在着消长关系。讨论了这2种温室气体排放的影响因素,并初步分析了它们对温室效应的相对贡献。     

大兴安岭重度火烧迹地天然次生林土壤温室气体通量及其影响因子

为研究大兴安岭重度火烧迹地自然恢复后的林分土壤温室气体源汇强度及其影响因素,采用静态箱/气相色谱法,对生长季(6—9月)天然次生林土壤温室气体CO₂、CH₄、N₂O通量进行原位观测.结果表明: 1)生长季内天然次生林土壤为大气CO₂、N₂O的源,CH₄的汇,平均通量分别为575.81 mg·m^-2·h^-1、17.81 μg·m^-2·h^-1和-68.69 μg·m^-2·h^-1;CO₂与CH₄通量在生长季内表现出明显的双峰变化规律,N₂O通量则呈单峰变化,且均在8月达到观测期的最大值.2)土壤温度是影响该区天然次生林土壤温室气体通量的主控因子,土壤湿度和大气湿度在昼夜与季节尺度上与土壤温室气体通量的相关性不同.3)该区天然次生林9:00—12:00时段观测获得的土壤气体通量值经矫正后可代表当日气体通量.研究补充了大兴安岭火烧迹地森林生态系统温室气体通量数据,为该区土壤温室气体源汇的相关研究提供了依据.     

甲烷排放部分抵消湿地生态系统碳汇功能：全球数据分析

湿地生态系统是吸收全球大气二氧化碳(CO₂)的汇,同时土壤厌氧环境造成其是大气甲烷(CH₄)的源。尽管有证据表明,湿地生态系统CH₄排放部分抵消其对大气CO₂的净吸收,但目前未见全球尺度湿地CH₄排放对其净生态系统CO₂交换(NEE)抵消效应的研究。本研究分析了全球内陆湿地(泥炭湿地和非泥炭湿地)以及滨海湿地(海草床、盐沼和红树林)中同时测定湿地NEE和CH₄排放通量的数据。结果表明：各类型湿地生态系统均为大气CO₂的汇,NEE值排序为红树林(-2011.0 g CO₂·m^-2·a^-1)<盐沼(-1636.6 g CO₂·m^-2·a^-1)<非泥炭地(-870.8 g CO₂·m^-2·a^-1)<泥炭地(...     

库布齐沙漠东部不同生物结皮发育阶段土壤温室气体通量

以流动沙地为对照,采用时空替代法分析库布齐沙漠东部固定沙地上不同发育阶段生物结皮藻类结皮和地衣结皮土壤温室气体通量特征及其与环境因子之间的关系,研究生物结皮发育对荒漠土壤温室气体通量的影响.结果表明: 荒漠土壤CO₂排放通量大小为地衣结皮(128.5 mg·m^-2·h^-1)>藻结皮(70.2 mg·m^-2·h^-1)>流动沙地(48.2 mg·m^-2·h^-1),CH₄吸收通量大小为地衣结皮(30.4 μg·m^-2·h^-1)>藻结皮(21.2 μg·m^-2·h^-1)>流动沙地(18.2 μg·m^-2·h^-1),N₂O排放通量大小为地衣结皮(6.6 μg·m^-2·h^-1)>藻结皮(5.4 μg·m^-2·h^-1)>流动沙地(2.5 μg·m^-2·h^-1).CO₂排放具有明显的季节变化,生长季显著大于非生长季;CH₄和N₂O季节变化差异不显著,前者生长季吸收大于非生长季,后者非生长季排放大于生长季.土壤有机碳和全氮含量、土壤微生物数量均是影响温室气体通量的重要因素,环境水热因子是影响土壤CO₂排放的关键因子,但CH₄和N₂O通量对水热因子的变化不敏感.随着植被恢复和生物结皮发育,荒漠土壤温室气体累积通量的不断增大导致其百年尺度的全球增温潜势亦显著提高,依次为地衣结皮(1135.7 g CO₂-e·m^-2·a^-1)>藻结皮(626.5 g CO₂-e·m^-2·a^-1) >流动沙地(422.7 g CO₂-e·m^-2·a^-1).     

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比,降低有机质的分解速率,增强了陆地生态系统对大气CO₂的固持作用;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,尚没有相关研究报道.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.     

Sn-S and Ru-Ru bonds cleavage reactions between [Ph3SnS(CH2)3SSnPh3] and Ru3(CO)12: X-ray crystal structures of [Ph3SnS(CH2)3SSnPh3] and trans-[Ru(CO)4(SnPh3)2]

The organotin complex [Ph₃SnS(CH₂)₃SSnPh₃] (1) was synthesized by PdCl₂ catalyzed reaction between Ph₃SnCl and disodium-1,3-propanedithiolate which in turn was prepared from 1,2-propanedithiol and sodium in refluxing THF. Reaction of 1 with Ru₃(CO)₁₂ in refluxing THF affords the mononuclear complex trans-[Ru(CO)₄(SnPh₃)₂] (2) and the dinuclear complex [Ru₂(CO)₆(μ-κ²-SCH₂CH₂CH₂S)] (3) in 20 and 11% yields, respectively, formed by cleavage of Sn-S bond of the ligand and Ru-Ru bonds of the cluster. Treatment of pymSSnPPh₃ (pymS = pyrimidine-2-thiolate) with Ru₃(CO)₁₂ at 55-60 °C also gives 2 in 38% yield. Both 1 and 2 have been characterized by a combination of spectroscopic data and single crystal X-ray diffraction analysis.     

Transesterification of sunflower oil to biodiesel on ZrO2 supported La2O3 catalyst

ZrO₂ supported La₂O₃ catalyst prepared by impregnation method was examined in the transesterification reaction of sunflower oil with methanol to produce biodiesel. It was found that the catalyst with 21 wt% loaded La₂O₃ and calcined at 600 °C showed the optimum activity. The basic property of the catalyst was studied by CO₂-TPD, and the results showed that the fatty acid methyl ester (FAME) yield was related to their basicity. The catalyst was also characterized by TG–DTA, XRD, FTIR, SEM and TEM, and the mechanism for the formation of basic sites was discussed. It was also found that the crystallite size of support ZrO₂ decreased by loading of La₂O₃, and the model of the solid-state reaction on the surface of La₂O₃/ZrO₂ catalyst was proposed. Besides, the influence of various reaction variables on the conversion was investigated.     

Glucose biosensor based on the room-temperature phosphorescence of TiO2/SiO2 nanocomposite

The direct immobilization of glucose oxidase (GOD) on TiO₂/SiO₂ nanocomposite and its application as glucose biosensor were investigated. The room-temperature phosphorescence of TiO₂/SiO₂ nanocomposite can be quenched by hydrogen peroxide (H₂O₂). The detection of glucose may be accomplished by monitoring the formation of hydrogen peroxide which generated in the oxidation process of glucose with the catalysis of GOD. To our surprise, by using a 96-hole polyporous plate accessory of fluorescence spectrophotometer, the biosensor exhibits excellent linear response to glucose concentrations ranging from 1.0 × 10⁻⁹ to 1.0 × 10⁻² M with a detection limit of 1.2 × 10⁻¹⁰ M. The TiO₂/SiO₂ nanocomposite can be used as both supporting material and signal transducer. The phosphorescence intensity and color of the biosensor change obviously and even could be observed with naked eyes by continuous addition of glucose. Based on the room-temperature phosphorescence of TiO₂/SiO₂ nanocomposite, a new method of solid substrate-room-temperature phosphorimetry (SS-RTP) for glucose determination is proposed. A glucose biosensor was fabricated with wide determination concentration range, low detection limit, high sensitivity, and fast response time. And the biosensor has been successfully applied to the determination of glucose in human blood serum. The coacervation of GOD enzyme and its interaction with TiO₂/SiO₂ nanocomposite enlarge the surface area and enhance the chemical stability of GOD. The nice biocompatibility, large surface area, good chemical stability and nontoxicity of the TiO₂/SiO₂ nanocomposite have made this material suitable for functioning as biosensor.     

Study on the heterogeneous degradation of chitosan with H2O2 catalyzed by a new supermolecular assembly crystal: [C6H8N2]6H3[PW12O40]·2H2O

A new supermolecular assembly crystal, [C₆H₈N₂]₆H₃[PW₁₂O₄₀]·2H₂O (DMB-PWA), was synthesized with phosphotungstic acid (PWA) and 1,2-diaminobenzene (DMB) under hydrothermal conditions and was characterized by Fourier-transform infrared spectra (FTIR) and single-crystal X-ray diffraction analysis. DMB-PWA could effectively catalyze oxidative degradation of chitosan with H₂O₂ in the heterogeneous phase. The optimum degradation conditions were determined by orthogonal tests as follows: amount of chitosan 1.00 g, 30% (wt %); H₂O₂, 3.0 mL; dosage of catalyst, 0.06 g; reaction temperature, 85 °C; and reaction time, 30 min. The water-soluble chitosan with a viscosity-average molecular weight (M_v) of 4900 was obtained under the optimum degradation conditions and was characterized by FTIR, ultraviolet-visible diffuse reflection spectra (UV-vis DRS), and X-ray powder diffraction analysis.     

血红蛋白A2现象发生机制的研究——“红细胞HbA2”为HbA2与HbA的结合产物

为了弄清血红蛋白A₂现象的发生机制,我们对“红细胞HbA₂”的化学组成进行了分析。“红细胞HbA₂”的双向电泳结果表明,它含有两种血红蛋白成分:一种相当于HbA,另一种很可能是溶血液HbA₂。其单向二次电泳结果也证明,它是由溶血液HbA₂和HbA所组成。结果初步说明,盘红细胞中HbA₂可能与HbA结合存在。两者可能有相互作用,也许这是产生血红蛋白A₂现象的原因。     

Kinetic studies of the reduction of hexaaquacobalt(III) perchlorate by a cobaloxime, [Co(dmgBF2)2(H2O)2]

The reaction of with Co(dmgBF₂)₂(H₂O)₂ in 1.0 M HClO₄/LiClO₄ was found to be first-order in both reactants and the [H⁺] dependence of the second-order rate constant is given by k_2obs = b/[H⁺], b at 25 °C is 9.23 ± 0.14 × 10² s⁻¹. The [H⁺] dependence at lower temperatures shows some saturation effect that allowed an estimate of the hydrolysis constant for as K_a = 9.5 × 10⁻³ M at 10 and 15 °C. Marcus theory and the known self-exchange rate constant for Co(OH₂)₅OH^2+/+ were used to estimate an electron self-exchange rate constant of k₂₂ = 1.7 × 10⁻⁴ M⁻¹ s⁻¹ for .     

On an erroneous view of fluxional behaviour of [Fe3(CO)12]

The idea that the mechanism of the very low energy fluxional behaviour of [Fe₃(CO)₁₂] may be based on the movement of the ligand icosahedron about the central Fe₃ triangle which corresponds to a rotational symmetry operation of the CO ligand icosahedron is discussed and rejected.     

Cobalt(III) complexes with linear hexadentate N6 or N4S2 donor set atoms providing pyridyl-amide-amine/thioether coordination

Two new cobalt(III) complexes of symmetric hexadentate ligand with N₆ [1,10-bis(2-picolinamide)-4,7-diazadecane (pycdpnen)] and N₄S₂ [1,8-bis(2-picolinamide)-3,6-dithiaoctane (pycdadt)] donor set atoms have been synthesized as perchlorate salts and characterized by spectroscopic methods. All two ligands with strong-field pyridylcarboxamido N donor stabilize Co(III) as demonstrated by the facile oxidation of the cobalt center. The structures of [Co(pycdpnenH₋₂)](ClO₄) (1) and [Co(pycdadtH₋₂)](ClO₄) · H₂O (2) investigated by COSY, HMBC, HMQC and NOESY NMR studies show that compounds 1 and 2 have the same geometrical configuration. The X-ray analysis reveals that complex 2 crystallizes in a orthorhombic space group Pccn. The cation [Co(pycdadtH₋₂)]⁺ is distorted octahedral with the two pyridyl groups in cis position.     

Interactions between TGF-β1 and TGF-β3 and their role in medial edge epithelium cell death and palatal fusion in vitro

In recent decades, studies have shown that both TGF-β₁ and TGF-β₃ play an important role in the induction of medial edge epithelium (MEE) cell death and palatal fusion. Many of these experiments involved the addition or blockage of one of these growth factors in wild-type (WT) mouse palate cultures, where both TGF-β₁ and TGF-β₃ are present. Few studies have addressed the existence of interactions between TGF-β₁ and TGF-β₃, which could modify their individual roles in MEE cell death during palatal fusion. We carried out several experiments to test this possibility, and to investigate how this could influence TGF-β₁ and TGF-β₃ actions on MEE cell death and palatal shelf fusion. We double-immunolabelled developing mouse palates with anti-TGF-β₁ or anti-TGF-β₃ antibodies and TUNEL, added rhTGF-β₁ or rhTGF-β₃ or blocked the TGF-β₁ and TGF-β₃ action at different concentrations to WT or Tgf-β₃ null mutant palate cultures, performed in situ hybridizations with Tgf-β₁ or Tgf-β₃ riboprobes, and measured the presence of TUNEL-positive midline epithelial seam (MES) cells and MES disappearance (palatal shelf fusion) in the different in vitro conditions. By combining all these experiments, we demonstrate great interaction between TGF-β₁ and TGF-β₃ in the developing palate and confirm that TGF-β₃ has a more active role in MES cell death than TGF-β₁, although both are major inductors of MES disappearance. Finally, the co-localization of TGF-β₁, but not TGF-β₃, with TUNEL in the MES allows us to suggest a possible role for TGF-β₁ in MES apoptotic clearance.     

Antibacterial properties of recombinant human non-pancreatic secretory phospholipase A2

Human non-pancreatic secretory phospholipase A₂ (hnpsPLA₂) is a group IIA phospholipase A₂ which plays an important role in the innate immune response. This enzyme was found to exhibit bactericidal activity toward Gram-positive bacteria, but not Gram-negative ones. Though native hnpsPLA₂ is active over a broad pH range, it is only highly active at alkaline conditions with the optimum activity pH of about 8.5. In order to make it highly active at neutral pH, we have obtained two hnpsPLA₂ mutants, Glu89Lys and Arg100Glu that work better at neutral pH in a previous study. In the present study, we tested the bactericidal effects of the native hnpsPLA₂ and the two mutants. Both native hnpsPLA₂ and the two mutants exhibit bactericidal activity toward Gram-positive bacteria. Furthermore, they can also kill Escherichia coli, a Gram-negative bacterium. The two mutants showed better bactericidal activity for E. coli at neutral pH than the native enzyme, which is consistent with the enzyme activities. As hnpsPLA₂ is highly stable and biocompatible, it may provide a promising therapy for bacteria infection treatment or other bactericidal applications.