Adsorption–Reduction Behavior of Co(NH3) on Activated Carbon

A novel method has been put forward to retrofit the wet ammonia desulfurization process to realize the combined removal of sulfur dioxide and nitric oxide by introducing soluble cobalt(II) salt into aqueous ammonia solution. The active constituent of scrubbing NO from the flue gases is the produced by ammonia coordinating with Co²⁺. The regeneration of can be realized under the catalysis of activated carbon so as to sustain a high NO removal efficiency for a long time. In this paper, the adsorption–reduction behavior of on activated carbon has been researched using scanning electron microscopy, X‐ray diffraction, and X‐ray photoelectron spectroscopy. A conclusion can be drawn from the results that cobalt ions in the aqueous solution are adsorbed by activated carbon and most of them are reduced to Co²⁺ ions, and some of the Co²⁺ ions are further reduced into metallic cobalt. The results also demonstrate that the functional groups on the surface of carbon take part in this redox reaction. The C? H groups on the carbon surface are oxidized into C? OH, and then some of the hydroxyl groups are further oxidized into carbonyl or carboxyl groups.     

二氧化碳相变技术应用于新型震源研发的可行性研究

为了研究二氧化碳物理相变技术应用于新型震源研发的可行性,在地下成层性较好的某煤田地震测区,开展了利用二氧化碳相变技术激发地震波的野外人工震源激发-接收实验.并与传统炸药震源进行了对比.地震数据利用Aries2.66型垂直分量反射地震仪和PDS-2型三分量地震仪接收.根据实测地震数据,从野外地震记录震相识别,初至波传播距离分析,震源近场地震信号时频分析,CO₂相变激发震源子波提取和基于CO₂震源子波的地震初至波波形反演实验等多个方面,进行了关于CO₂相变激发技术能否产生地震波信号以及能否将其应用于新型震源研发的可行性研究.研究结果表明CO₂物理相变膨胀能够产生能量集中的地震波信号;在实验区地质条件和激发参量下地震记录中初至波的可识别的传播距离约为1 km;震源近场地震信号的主频集中在8~13 Hz;利用震源近场数据提取了CO₂震源子波;通过地震初至波波形反演实验认为这种震源子波能够应用于波形反演等方面的研究.因为CO₂相变激发具有绿色、环保、安全等方面的优点,若能进一步在激发能量、激发—延迟时间一致性等方面加以改进,该技术有望在城市隐伏活动断层探测、城市地下空间探测、煤矿高瓦斯环境人工地震勘探等领域发挥重要的作用.

     

fCO2 variability in the Bay of Biscay during ECO cruises

The Bay of Biscay is part of the North Atlantic Ocean, the most important sink of CO₂, and a subduction zone of mode waters that favours the entry of carbon to the ocean interior. To investigate the seasonal and interannual variability of CO₂ uptake, continuous underway measurements of the partial pressure of CO₂ at sea surface were performed along a commercial route between Vigo (Spain) and St. Nazaire (France). An unattended measuring system of CO₂ fugacity (fCO₂), with meteorological station, and temperature, salinity, oxygen and fluorescence sensors, was installed on board of ships of opportunity (RO-RO L’Audace and RO-RO Surprise).     

Degassing patterns of Tungurahua volcano (Ecuador) during the 1999–2006 eruptive period,inferred from remote spectroscopic measurements of SO2 emissions

This paper presents the results of 7 years (Aug. 1999–Oct. 2006) of SO₂ gas measurements during the ongoing eruption of Tungurahua volcano, Ecuador. From 2004 onwards, the operation of scanning spectrometers has furnished high temporal resolution measurements of SO₂ flux, enabling this dataset to be correlated with other datasets, including seismicity. The emission rate of SO₂ during this period ranges from less than 100 to 35,000 tonnes/day (t d^− 1) with a mean daily emission rate of 1458 t d^− 1 and a standard deviation of ± 2026 t d^− 1. Average daily emissions during inferred explosive phases are about 1.75 times greater than during passive degassing intervals. The total amount of sulfur emitted since 1999 is estimated as at least 1.91 Mt, mostly injected into the troposphere and carried westwards from the volcano. Our observations suggest that the rate of passive degassing at Tungurahua requires SO₂ exsolution of an andesitic magma volume that is two orders of magnitude larger than expected for the amount of erupted magma. Two possible, and not mutually exclusive, mechanisms are considered here to explain this excess degassing: gas flow through a permeable stagnant-magma-filled conduit and gas escape from convective magma overturning in the conduit. We have found that real-time gas monitoring contributes significantly to better eruption forecasting at Tungurahua, because it has provided improved understanding of underlying physical mechanisms of magma ascent and eruption.     

Role of carbon dioxide in the dynamics of magma ascent in explosive eruptions

 The role of carbon dioxide in the dynamics of magma ascent in explosive eruptions is investigated by means of numerical modeling. The model is steady, one-dimensional, and isothermal; it calculates the separated flow of gas and a homogeneous mixture of liquid magma and crystals. The magma properties are calculated on the basis of magma composition and crystal content and are allowed to change along the conduit due to pressure decrease and gas exsolution. The effect of the presence of a two-component (water + carbon dioxide) exsolving gas phase is investigated by performing a parametric study on the CO₂/(H₂O+CO₂) ratio, which is allowed to vary from 0 to 0.5 at either constant total volatile or constant water content. The relatively insoluble carbon dioxide component plays an important role in the location of the volatile-saturation and magma-fragmentation levels and in the distribution of the flow variables in the volcanic conduit. In detail, the results show that an increase of the proportion of carbon dioxide produces a decrease of the mass flow rate, pressure, and exit mixture density, and an increase of the exit gas volume fraction and depth of the fragmentation level. A relevant result is the different role played by water and carbon dioxide in the eruption dynamics; an increasing amount of water produces an increase of the mass flow rate, and an increasing amount of carbon dioxide produces a decrease. Even small amounts of carbon dioxide have major consequences on the eruption dynamics, implying that the multicomponent nature of the volcanic gas must be taken into account in the prediction of the eruption scenario and the forecasting of volcanic hazard. Received: 6 March 1998 / Accepted: 28 October 1998     

The Role of Multiphase Chemistry in the Oxidation of Dimethylsulphide (DMS). A Latitude Dependent Analysis

A kinetic model for the OH-initiated homogeneous gas phase oxidation of dimethylsulfide (DMS) in the atmosphere (Saltelli and Hjorth, 1995), has been extended here to include the liquid phase chemistry. The updated model has then been employed to predict the temperature dependency of the MSA/nss-SO42- ratio. Model predictions have been compared with observational data reported in Bates et al. (1992). Sensitivity and uncertainty analysis has been performed in a Monte Carlo fashion to identify which are the important uncertainties on the input parameters and which are the possible combinations of parameter values that could explain the field observations. Results of the analysis have indicated that the temperature dependencies of the interactions between gas phase and liquid phase chemistry may to a large extent explain the observed T-dependence of the MSA/nss- SO42- ratio. The potential role of multi-phase atmospheric chemistry, not only in the case of SO2 but also of other oxidation products of DMS and, particularly, of DMS itself, has been highlighted.     

Short-Term Variability of Atmospheric DMS and Its Oxidation Products at Amsterdam Island during Summer Time

A one-month experiment was performed at Amsterdam Island in January 1998, to investigate the factors controlling the short-term variations of atmospheric dimethylsulfide (DMS) and its oxidation products in the mid-latitudes remote marine atmosphere. High mixing ratios of DMS, sulfur dioxide (SO₂) and dimethylsulfoxide (DMSO) have been observed during this experiment, with mean concentrations of 395 parts per trillion by volume (pptv) (standard deviation, = 285, n = 500), 114 pptv ( = 125, n = 12) and 3 pptv ( = 1.2, n = 167), respectively. Wind speed and direction were identified as the major factors controlling atmospheric DMS levels. Changes in air temperature/air masses origin were found to strongly influence the dimethylsulfoxide (DMSO)/DMS and SO₂/DMS molar ratios, in line with recent laboratory data. Methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO₄ ^2–) mean concentrations in aerosols during this experiment were 12.2± 6.5 pptv (1, n=47) and 59 ± 33 pptv (1, n=47), respectively. Evidence of vertical entrainment was reported following frontal passages, with injection of moisture-poor, ozone-rich air. High MSA/ nss-SO₄ ^2– molar ratios (mean 0.44) were calculated during these events. Finally following frontal passages, few spots in condensation nuclei (CN) concentration were also observed.     

The Validity of Similarity Theory in the Roughness Sublayer Above Forests

Flux-gradient relationships based upon similarity theory have been reported to severely underestimate scalar fluxes in the roughness sublayer above forests, as compared to independent flux estimates (for example, eddy covariance or energy balance measurements). This paper presents the results of a unique three-month investigation into the validity of similarity theory in the roughness sublayer above forests. Eddy covariance and flux-gradient measurements of carbon dioxide (CO²) exchange were compared above a mixed deciduous forest at Camp Borden, Ontario, both before and after leaf senescence. The eddy covariance measurements used a Li-Cor infrared gas analyzer, and the flux-gradient (similarity theory) measurements featured a tunable diode laser Trace Gas Analysis System (TGAS). The TGAS resolved the CO² concentration difference to 300 parts per trillion by volume (ppt) based upon a half-hour sampling period. The measured enhancement factor (the ratio of independent flux estimates, in this case eddy covariance, to similarity theory fluxes) was smaller and occurred closer to the canopy than in most previous investigations of similarity theory. Very good agreement between the eddy covariance and similarity theory fluxes was found between 1.9 and 2.2 canopy heights (h^c), and the mean enhancement factors measured before and after leaf senescence were 1.10 plusmn; 0.06 and 1.24 ± 0.07, respectively. Larger discrepancies were measured closer to the canopy (1.2 to 1.4 h^c), and mean enhancement factors of 1.60 ± 0.10 and 1.82 ± 0.11 were measured before and after leaf senescence, respectively. Overall, the Borden results suggest that similarity theory can be used within the roughness sublayer with a greater confidence than previously has been believed.     

MIPAS-Transall Observations of the Variability of CLONO2 during the Arctic Winter of 1994/95

In the winter of 1994/95 the German Transall research aircraft performed 5 campaigns in the European Arctic with 22 flights altogether. An extensive dataset of HNO3, ClONO2 and O3 column amounts was obtained by MIPAS-FT (Michelson Interferometer for Passive Atmospheric Sounding - Flugzeug Transall) onboard the aircraft. In this paper we present the variability of the ClONO2 reservoir gas in the course of the winter. We include groundbased FTIR measurements of HF, HCl and ClONO2 to discuss the airborne observations with regard to the partitioning of inorganic chlorine.From mid-December until the end of January, MIPAS measured a stable ClONO2 collar with constantly low column amounts inside the polar vortex and maxima at the edge. This observation reflected widespread conversion of ClONO2 to reactive chlorine inside the vortex for at least six weeks. In good accordance, the ground stations measured low in-vortex HCl and ClONO2 column amounts and conversion of HCl into ClONO2 in the region of the ClONO2 maxima. In the first week of February the ClONO2 amounts started to increase in the edge region as well as inside the vortex. Between March 21 and 27, just one week after the last cold period, MIPAS observed exclusively high ClONO2 column amounts inside the vortex, indicating fast deactivation of active chlorine. In the same period the ground stations measured an excess of ClONO2 over HCl. Further, the high ClONO2 implies that the polar vortex was renoxified in March. Lower ClONO2 values, observed inside the vortex on the flights of April 5 and 8, and an increased HCl/ClONO2 ratio, measured from ground, marked the starting redistribution within the chlorine reservoir species to the photochemically more stable HCl.In February, March and April, MIPAS observed mixing of ClONO2-rich air masses with midlatitude air at the vortex edge. A very clear event happened on March 27. On this flight a distinct ClONO2 minimum was measured at the vortex edge, which was closely correlated with a filament of midlatitude air observed by OLEX (Ozone Lidar EXperiment) onboard the Transall.     

半干旱地区地气界面水汽和二氧化碳通量的日变化及季节变化

采用涡动相关方法连续观测2002年10月到2003年12月半干旱地区地气界面水汽和二氧化碳通量变化,分析水汽和二氧化碳通量的季节和日变化规律,同时比较农田和退化草地两种不同下垫面物质和能量通量交换过程的差异,得到如下一些主要结果:(1)半干旱地区湿季,相距5 km的两种不同下垫面,即使在同一天气过程控制下,不同植被下垫面的降雨分布仍不尽相同,甚至相差很大.这表明降雨空间的分布是很不均匀的,具有很强的局地特征.(2)在干季近地面层能量收支中,两种不同下垫面上的有效能量(净辐射与地表热流量之差)主要分配为感热通量,潜热通量在非生长季(干季)通常很小.在湿季(生长季),潜热通量与感热通量相当,但农田下垫面的潜热通量大于退化草原下垫面.(3)土壤的温度和湿度日变化主要集中在0～20 cm土壤层内,在湿季农田下垫面土壤的湿度有明显的跳跃,这与降雨过程有很好的相关.(4)在非生长季,两种不同下垫面地气间二氧化碳通量差别不大,都很小.白天由于光合作用,在生长季农田下垫面吸收CO2通量较退化草原大,但比湿润地区稻田下垫面小一个量级,远小于森林生态系统.