Study on the failure mechanism of potassium-based sorbent for CO2 capture and the improving measure

With thermogravimetric apparatus (TGA), X-ray diffraction (XRD) and barium sulfate gravimetric methods, the carbonation reactivities of K₂CO₃ and K₂CO₃/Al₂O₃ in the simulated flue gases with SO₂ are investigated and the reaction equations are inferred. Results show that there are KHCO₃ and K₂SO₃ generated. The generation K₂SO₃ reduces the utilization ratio of the sorbent. H₂O may accelerates the sulfation reaction of AR K₂CO₃ as K₄H₂(CO₃)₃·1.5H₂O is generated in the reaction among K₂CO₃, SO₂ and H₂O. K₂SO₃ is directly generated from sulfation reaction of K₂CO₃/Al₂O₃, because there are K₂CO₃·1.5H₂O and K₂SO₃ generated in the reaction among K₂CO₃/Al₂O₃, SO₂ and H₂O. K₂CO₃·1.5H₂O does not react with SO₂, and K₂CO₃·1.5H₂O/Al₂O₃ reacts with SO₂ slowly. Compare with the reaction process without H₂O pretreatment, the reaction rates of KAl30 increased after H₂O pretreatment and the failure ratio is about a half of that without H₂O pretreatment. So, K₂CO₃/Al₂O₃ shows good carbonation and anti-sulfation characteristic after H₂O pretreatment.     

我国大气细颗粒物污染防治目标和控制措施研究

我国面临着严重的细颗粒物(PM2.5)污染问题,PM2.5对人体健康、能见度、气候变化、生态系统等均产生了不良影响。本文旨在提出我国PM2.5污染防治目标和控制措施,为从根本上改善空气质量提供科学依据。首先,本文提出了2020年和2030年我国PM2.5污染防治目标。其次,采用能源和污染排放技术模型,分情景预测了我国未来一次大气污染物排放量的变化趋势。基于情景预测结果和此前研究建立的一次污染物排放与PM2.5浓度间的非线性关系,确定了2020年—2030年与PM2.5浓度改善相适应的全国和重点区域大气污染物减排目标。最后,利用能源和污染排放技术模型,提出了实现大气污染物减排的技术措施和对策建议。研究表明,2030年全国二氧化硫、氮氧化物、一次PM2.5和挥发性有机物的排放量应分别比2012年至少削减51%、64%、53%和36%,氨排放量也要略有下降。对于污染严重的重点区域,必须采取更严格的控制力度。要实现上述减排,应加快能源结构调整,推进煤炭清洁高效集中可持续利用,建立"车-油-路"一体的移动源控制体系,并强化多源多污染物的末端控制。     

Emission of CO2, CH4 and N2O from freshwater marsh in northeast of China

The wetlands play an important role in carbon storage, especially at high latitudes, at which they store nearly one-third of global soil carbons. However, few studies have investigated the emissions of CO(2), CH(4) and N(2)O in the long-term, especially effects of freeze-thaw cycles on these gases emissions in freshwater marsh ecosystems. In this paper, we collected greenhouse gas emission data from a freshwater marsh area in China for 4 years, evaluated their release variables and speculated on their potential atmospheric impact. For this paper, we report on the CO(2), CH(4) and N(2)O emission rates recorded from June 2002 to November 2005 in the Sanjiang Plain of northeast China. We measured their interannual variations and fluctuations, as well as factors affecting their emissions, and estimated their regulation and freeze-thaw cycle impacts. Our results revealed obvious CO(2) and CH(4) emission fluctuations during the winter months, and during the freeze-thaw cycle, and a strong interannual variation during the growing season. Overall, we documented a close relationship between the CO(2) and CH(4) emissions, implicating some regulatory commonality. We determined that the marsh was a N(2)O sink during the winter, but a significant source of N(2)O during the freeze-thaw cycle as the temperature increased, especially in early summer. During the thaw-freeze period, the N(2)O levels were positively correlated with the water depth. Additionally, water depth greatly governed the interannual variation of the N(2)O emissions from the marshes during the thaw-freeze period.     

Performance of lime-BHA solidified plating sludge in the presence of Na2SiO3 and Na2CO3

This research investigated the performance of lime-BHA (black rice husk ash) solidified plating sludge with 2 wt% NaO from Na(2)SiO(3) and Na(2)CO(3) at the level of 0, 30 and 50 wt%. The sludge was evaluated for strength development, leachability, solution chemistry and microstructure. The lime-BHA solidified plating sludge with Na(2)SiO(3) and Na(2)CO(3) had higher early strength when compared to the control. The addition of Na(2)SiO(3) and Na(2)CO(3) increased the OH(-) concentration and decreased the Ca(2+) and heavy metal ions in solution after the first minute. The XRD patterns showed that the addition of Na(2)SiO(3) resulted in the formation of calcium silicate hydrates, while the addition of Na(2)CO(3) resulted in CaCO(3). The heavy metals from the plating sludge, especially Zn, were immobilized in calcium zincate and calcium zinc silicate forms for the lime-BHA with and without Na(2)SiO(3) solidified wastes, while samples with Na(2)CO(3) contained Zn that was fixed in the form of CaZnCO(3). The cumulative leaching of Fe, Cr and Zn from the lime-BHA solidified plating sludge decreased significantly when activators were added, especially Na(2)CO(3).     

Model prediction on the rise of pCO2 in uniform flows by leakage of CO2 purposefully stored under the seabed

A numerical study was conducted to predict pCO₂ change in the ocean on a continental shelf by the leakage of CO₂, which is originally stored in the aquifer under the seabed, in the case that a large fault connects the CO₂ reservoir and the seabed by an earthquake or other diastrophism. The leakage rate was set to be 6.025 × 10⁻⁴ kg/m²/sec from 2 m × 100 m fault band, which corresponds to 3800 t-CO₂/year, referring to the monitored seepage rate from an existing EOR field. The target space in this study was limited to the ocean above the seabed, the depth of which was 200 or 500 m. The computational domain was idealistically rectangular with the seabed fault-band perpendicular to the uniform flow. The CO₂ takes a form of bubbles or droplets, depending on the depth of water, and their behaviour and dissolution were numerically simulated during their rise in seawater flow. The advection–diffusion of dissolved CO₂ was also simulated. As a result, it was suggested that the leaked CO₂ droplets/bubbles all dissolve in the seawater before spouting up to the atmosphere, and that the increase in pCO₂ in the seawater was smaller than 500 μ atm.     

Photocatalytic Production of Methane and Hydrogen Through Reduction of Carbon Dioxide with Water Using Titania Pellets

This paper presents an experimental study on employing a pellet form of catalyst in photo-reduction of carbon dioxide with water. Water was first absorbed into titania pellets. Highly purified carbon dioxide gas was then discharged into a reactor containing the wet pellets, which were then illuminated continuously for 65 hours using UVC lamps. Analysing the products accumulated in the reactor confirmed that methane and hydrogen were produced through photo-reduction of carbon dioxide with water. No other hydrocarbons were detected. Increasing the temperature in the reactor has showed little change on the amount of methane produced.     

The direct influence of ship traffic on atmospheric PM2.5, PM10 and PAH in Venice

The direct influence of ship traffic on atmospheric levels of coarse and fine particulate matter (PM_2.5, PM₁₀) and fifteen polycyclic aromatic hydrocarbons (PAHs) has been estimated in the urban area of Venice. Data analysis has been performed on results collected at three sites over the summer, when ship traffic is at a maximum. Results indicate that monitoring of the PM daily concentrations is not sufficiently detailed for the evaluation of this contribution, even though it could be useful for specific markers such as PAHs. Therefore a new methodology, based on high temporal resolution measurements coupled with wind direction information and the database of ship passages of the Harbour Authority of Venice has been developed. The sampling sites were monitored with optical detectors (DustTrack^® and Mie pDR-1200) operating at a high temporal resolution (20s and 1s respectively) for PM_2.5 and PM₁₀. PAH in the particulate and gas phases were recovered from quartz fibre filters and polyurethane foam plugs using pressurised solvent extraction, the extracts were then analysed by gas chromatography- high-resolution mass spectrometry. Our results shows that the direct contribution of ships traffic to PAHs in the gas phase is 10% while the contribution to PM_2.5 and to PM₁₀ is from 1% up to 8%.     

Decomposition of NaBH4 with self-regeneration of carbon-supported CoCl2 catalyst

In this study, economically favorable CoCl₂ catalysts at four different amounts were supported on activated carbon (AC) for NaBH₄ dehydrogenation. Supported catalyst could achieve hydrogen release for 2,060 cycles, which is equivalent to 103 days of uninterrupted operation. Slow and continuous hydrogen release was observed in all experiments. Even 1 g of NaBH₄ can carry 1.2 L of hydrogen, and in hydrolysis process, it liberates 2.5 L of hydrogen that indicates the decomposition of water. EDX analysis and reverse burette measurements show that CoCl₂ could be homogeneously distributed on and permanently joined to the support surface. Kinetic investigation of the dehydrogenation reaction fits zero order kinetics, and activation energy was calculated to be 48 kJ/mol.     

Advanced oxidation treatment of pulp mill effluent for TOC and toxicity removals

Pulp mill effluent was treated by different advanced oxidation processes (AOPs) consisting of UV, UV/H2O2, TiO2-assisted photo-catalysis (UV/TiO2) and UV/H2O2/TiO2 in lab-scale reactors for total organic carbon (TOC) and toxicity removals. Effects of some operating parameters such as the initial pH, oxidant and catalyst concentrations on TOC and toxicity removals were investigated. Almost every method resulted in some degree of TOC and toxicity removal from the pulp mill effluent. However, the TiO2-assisted photo-catalysis (UV/TiO2) resulted in the highest TOC and toxicity removals under alkaline conditions when compared with the other AOPs tested. Approximately, 79.6% TOC and 94% toxicity removals were obtained by the TiO2-assisted photo-catalysis (UV/TiO2) with a titanium dioxide concentration of 0.75gl(-1) at pH 11 within 60min.     

深圳大气污染特征模拟及环境容量估算

本文根据深圳市8 个监测站点2013 年的逐日PM₁₀ 和PM_2.5 浓度监测数据、气象数据,统计风向、风速、稳定度联合频率等,利用污染物在大气中输送扩散模式,由实测的浓度值反推出污染物的产生量或排放量的方法,重点分析龙华新区PM₁₀ 和PM_2.5 的污染特征,并依据环境目标值,估算该区域剩余环境容量。研究结果表明,龙华新区全年盛行东风、南风,其风频分别为16.7%、13.2%,风速约为1.6m/s,PM₁₀、PM_2.5 浓度均呈现出季节性变化,秋、冬季浓度值较高,尤其在10 月到次年1 月份,其排放强度主要受本地污染源的影响。除此以外,其西、北部的污染源对其污染物浓度有一定的影响。新区PM₁₀ 和PM_2.5 的剩余环境容量均呈现负值,尤其以PM_2.5 最为突出,须大力加强减排控制,以达到环境目标值     

Size distributions of fine and ultrafine particles in the city of Strasbourg: correlation between number of particles and concentrations of NO(x) and SO(2) gases and some soluble ions concentration determination

An Electrical Low Pressure Impactor (ELPI) was used during spring and autumn 2003 in the centre of Strasbourg for the measurement of atmospheric aerosols size distribution. The concentration of NO(x) and SO(2) in air was simultaneously measured with specific analysers. Samples were collected in the range 0.007-10 microm in equivalent aerodynamic diameter size. Number distributions are representative of a pollution originating from urban traffic with a particle size distribution exhibiting a nucleation mode below 29 nm and an accumulation mode around 80 nm in size. A mean particle density equal to 39000+/-35000 total particles per cm(3) with a size ranging from 7 to 10 microm was obtained after a sampling period of 2 weeks in spring. About 86.9% of the number of particles have an aerodynamic diameter below 0.1 microm and 13.1% between 0.1 and 1 microm. Correlation coefficients between the number of particles impacted on each ELPI plate and gas concentrations (SO(2) and NO(x)) showed that the numbers of particles with diameter between 0.10 and 0.62 microm are highly related to the NO(x) concentration. This result indicates that particles are traffic induced since NO(x) is mainly emitted by cars as shown by measurements on various sites. Particles are less clearly correlated to the SO(2) concentration. Particle analysis on different ELPI plates for a sampling period of 2 weeks in autumn showed high level of soluble NO(3)(-), SO(4)(2-) and NH(4)(+) ions. Indeed, up to 90% b.w. of these three species were found in the particle range 0.1-1 microm. The formation of particulate NH(4)NO(3) is favoured by high NO(x) concentration, which induces the formation of gaseous HNO(3).     

Using Sediment Budgets to Investigate the Pathogen Flux Through Catchments

We demonstrate a materials budget approach to identify the main source areas and fluxes of pathogens through a landscape by using the flux of fine sediments as a proxy for pathogens. Sediment budgets were created for three subcatchment tributaries of the Googong Reservoir in southeastern New South Wales, Australia. Major inputs, sources, stores, and transport zones were estimated using sediment sampling, dam trap efficiency measures, and radionuclide tracing. Particle size analyses were used to quantify the fine-sediment component of the total sediment flux, from which the pathogen flux was inferred by considering the differences between the mobility and transportation of fine sediments and pathogens. Gullies were identified as important sources of fine sediment, and therefore of pathogens, with the pathogen risk compounded when cattle shelter in them during wet periods. The results also indicate that the degree of landscape modification influences both sediment and pathogen mobilization. Farm dams, swampy meadows and glades along drainage paths lower the flux of fine sediment, and therefore pathogens, in this landscape during low-flow periods. However, high-rainfall and high-flow events are likely to transport most of the fine sediment, and therefore pathogen, flux from the Googong landscape to the reservoir. Materials budgets are a repeatable and comparatively low-cost method for investigating the pathogen flux through a landscape.     

Responses of Three Heathland Shrubs to Single or Repeated Experimental Trampling

In the last few decades, trampling has become a cause of major disturbance to natural areas. Trampling can occur regularly either seasonally or throughout the year, or as a single impact depending on a recreational activity or an event. This study, carried out on a coastal heathland in north Brittany (France), was based on the hypothesis that the vegetation response can differ depending on whether the trampling is repeated or due to a single event. The aim was to compare the resistance and the short-term recovery capacity of selected species in coastal heathland communities subjected to a trampling experiment, applied once or five times (with equal total number of passes from 0 to 800). The temporal distribution of the trampling did not affect the response of Erica ciliaris, whereas for Erica cinerea and Ulex gallii, trampling was slightly less damaging when applied once rather than five times. These differences could be linked to the lower resistance and the higher recovery capacity of E. ciliaris, compared with the two other species. This study also emphasized the influence of site location by comparing observations with previous studies. Plant resistance calculated here appeared to be lower than that calculated for a less stressful site. The relationship between plant traits and response to trampling was also investigated. The effects of the different times between disturbance application and observations of the short-term response of woody vegetation to experimental trampling is also discussed.     

Control of combustion-generated nitrogen oxides by selective non-catalytic reduction

Controlling nitrogen oxides (NO(x)) emissions is becoming a daunting technical challenge as increasingly strict emission limits are being imposed. The stringent regulations have prompted the innovation and characterization of NO(x) control technologies suitable for various applications. This paper presents a review on NO(x) removal techniques with particular reference to selective non-catalytic reduction (SNCR) technology. This includes initially how SNCR emerged as a technology along with a comparison with other relevant technologies. A review of various features related to selective non-catalytic gas phase injection of ammonia and ammonium salts (as reducing agent) is presented. The use of urea solution as a reducing agent and its performance in laboratory and pilot scale tests as well as large-scale applications is also discussed. Use of cyanuric acid as a potential reducing agent is also presented. The underlying reaction mechanisms have been reviewed for ammonia, urea and cyanuric acid for the explanation of various observations. Computational fluid dynamics (CFD) modeling as applied to SNCR is also presented. Subsequently the use of SNCR coupled with other in-combustion and post-combustion NO(x) control techniques is elaborated. Additionally, a two-stage NO(x) removal strategy to control un-reacted ammonia slip and to improve overall efficiency is discussed. At the end a summary is given which highlights various areas needing further research.     

Photo-oxidation of NO using an exterior paint--screening of various commercial titania in powder pressed and paint films

The present work aims to evaluate the photocatalytic activity of photo-TiO(2) from various producers (Evonik, Kemira, Kronos, Millennium, Sachtleben and Tayca), in the form of powder pressed films and upon incorporation in a water-based paint, for outdoor NO abatement. The photocatalytic activity of the different samples was evaluated in terms of NO conversion and selectivity towards nitrite and nitrate ions following approximately the ISO 22197-1:2007(E) standard. The highest yields obtained for powder pressed films were achieved with VLP7000 (0.70), followed by VLP7101 (0.55) and UVLP7500 (0.55), all from Kronos. On the other hand, when incorporated in paint films, the highest yields were obtained with PC500 and PC105 from Millennium and UV100 from Sachtleben (ca. 0.15). The paint matrix plays an important role on the photocatalytic activity. In particular, the time for steady state is one or two orders of magnitude higher when the photocatalysts are incorporated in paint films in relation to the powder pressed films. The paint films were activated following the procedure recommended by the above-mentioned standard. However, the photocatalytic activity of films incorporating P25 (Evonik) was displayed only when higher power radiation and higher humidity conditions were used. This allowed for similar levels of photocatalytic activity as the other paint films.     

Effect of oxygenated liquid additives on the urea based SNCR process

An experimental investigation was performed to study the effect of oxygenated liquid additives, H₂O₂, C₂H₅OH, C₂H₄(OH)₂ and C₃H₅(OH)₃ on NO_x removal from flue gases by the selective non-catalytic reduction (SNCR) process using urea as a reducing agent. Experiments were performed with a 150 kW pilot scale reactor in which a simulated flue gas was generated by the combustion of methane operating with 6% excess oxygen in flue gases. The desired levels of initial NO_x (500 ppm) were achieved by doping the fuel gas with ammonia. Experiments were performed throughout the temperature range of interest, i.e. from 800 to 1200 °C for the investigation of the effects of the process additives on the performance of aqueous urea DeNO_x. With H₂O₂ addition a downward shift of 150 °C in the peak reduction temperature from 1130 to 980 °C was observed during the experimentation, however, the peak reduction efficiency was reduced from 81 to 63% when no additive was used. The gradual addition of C₂H₅OH up to a molar ratio of 2.0 further impairs the peak NO_x reduction efficiency by reducing it to 50% but this is accompanied by a downward shift of 180 °C in the peak reduction temperature. Further exploration using C₂H₄(OH)₂ suggested that a 50% reduction could be attained for all the temperatures higher than 940 °C. The use of C₃H₅(OH)₃ as a secondary additive has a significant effect on the peak reduction efficiency that decreased to 40% the reductions were achievable at a much lower temperature of 800 °C showing a downward shift of 330 °C.     

关于“十四五”大气环境管理重点的思考

"十四五"是衔接我国"两个一百年"奋斗目标、开启全面建设社会主义现代化国家新征程的第一个五年,"十四五"的大气环境管理需要指向新的目标,同时面临新的挑战。本文通过梳理我国2013年以来大气环境质量改善效果,分析目前大气环境质量的差距,从推进中长期大气环境质量持续改善的视角,研究提出了"十四五"期间关于大气环境管理的定位和相关工作目标,并从完善大气环境管理体系、全面推进结构调整等方面,提出了对"十四五"大气环境管理重点工作的建议。     

减污降碳协同增效的关键路径与政策研究

全面推动实现减污降碳协同增效是新发展阶段我国兑现碳达峰碳中和庄严承诺、深入打好污染防治攻坚战、建设美丽中国的必然要求。环境污染物与二氧化碳排放的高度同源性是实现减污降碳协同增效的理论基础。本文首先就目标指标、管控区域、控制对象、措施任务、政策工具五个方面的协同性系统讨论了减污降碳协同增效的基本内涵。其次，着眼于当前大气环境治理与碳减排在中国的重要性，本文在国家层面讨论了二者的中长期协同控制路线图，阐述了重点协同区域的识别方法和重点部门的协同治理思路，系统提出了大气环境治理与碳减排的协同路径。再次，本文还就“无废城市”建设和生态保护这两个领域与碳减排的协同治理思路展开分析讨论。最后，针对减污降碳协同治理对政策体系的需求，提出了统筹优化减污降碳协同目标、建立协同法规标准、建立减污降碳协同管理制度三个方面的建议。本研究将有助于厘清各方对减污降碳协同增效的认识，对各级政府后续推进减污降碳协同治理工作提供理论和科学基础。     

Effects of nano-SiO(2) and different ash particle sizes on sludge ash-cement mortar

The effects of nano-SiO₂ on three ash particle sizes in mortar were studied by replacing a portion of the cement with incinerated sewage sludge ash. Results indicate that the amount of water needed at standard consistency increased as more nano-SiO₂ was added. Moreover, a reduction in setting time became noticeable for smaller ash particle sizes. The compressive strength of the ash–cement mortar increased as more nano-SiO₂ was added. Additionally, with 2% nano-SiO₂ added and a cure length of 7 days, the compressive strength of the ash–cement mortar with 1 μm ash particle size was about 1.5 times better that of 75 μm particle size. Further, nano-SiO₂ functioned to fill pores for ash–cement mortar with different ash particle sizes. However, the effects of this pore-filling varied with ash particle size. Higher amounts of nano-SiO₂ better influenced the ash–cement mortar with larger ash particle sizes.     

Ecological Impact Assessment in Data-Poor Systems: A Case Study on Metapopulation Persistence

Legislation on the protection of biodiversity (e.g., European Union Habitat and Bird Directives) increasingly requires ecological impact assessment of human activities. However, knowledge and understanding of relevant ecological processes and species responses to different types of impact are often incomplete. In this paper we demonstrate with a case study how impact assessment can be carried out for situations where data are scarce but some expert knowledge is available. The case study involves two amphibian species, the great crested newt (Triturus cristatus) and the natterjack toad (Bufo calamita) in the nature reserve the Meinweg in the Netherlands, for which plans are being developed to reopen an old railway track called the Iron Rhine. We assess the effects of this railway track and its proposed alternatives (scenarios) on the metapopulation extinction time and the occupancy times of the patches for both species using a discrete-time stochastic metapopulation model. We quantify the model parameters using expert knowledge and extrapolated data. Because of our uncertainty about these parameter values, we perform a Monte Carlo uncertainty analysis. This yields an estimate of the probability distribution of the model predictions and insight into the contribution of each distinguished source of uncertainty to this probability distribution. We show that with a simple metapopulation model and an extensive uncertainty analysis it is possible to detect the least harmful scenario. The ranking of the different scenarios is consistent. Thus, uncertainty analysis can enhance the role of ecological impact assessment in decision making by making explicit to what extent incomplete knowledge affects predictions.