我国大气环境管理历程与展望

随着大气环境问题从煤烟型向以PM_2.5和O₃为特征的区域复合型污染演变，我国大气污染控制模式从以污染物排放浓度控制为核心、以污染物排放总量控制为核心逐渐走向以大气环境质量改善为核心。特别是近几年，全国各地在空气质量管理、科学精准治污等领域开展一系列积极的探索与实践，取得了显著成效。本文系统回顾了近50年来我国不同阶段大气环境管理工作的特点，重点梳理了2013年《大气污染防治行动计划》实施以来，空气质量管理经验与成绩，结合减污降碳总体部署对我国2035年“美丽中国建设目标基本实现”时的空气质量进行了展望，从PM_2.5与O₃协同控制的角度出发，提出了“十四五”期间我国大气环境管理的总体思路。     

基于EKC的全面小康中国与发达国家环境质量比较

以2020年全面建成小康社会目标为依据,比较了我国2020年与主要发达国家同等经济水平阶段在能源消耗、大气环境、水环境等方面的差距。研究发现:主要发达国家环境质量拐点出现在20世纪70年代末到80年代初,人均GDP在1.4万~1.5万美元左右。人均GDP在1.1万~1.2万美元阶段时,我国大气污染物排放强度低于发达国家,但大气环境质量差于发达国家;主要水污染排放量高于主要发达国家,但水环境质量基本可达到发达国家同期水平。建议要正确认识环境与经济之间的EKC曲线关系,制定具有中国特色的环境问题解决路线图,提出具有阶段性、差异化、适度超前的环境质量目标。     

上海市近年来大气环境质量变化趋势分析

为了解上海市大气环境的状况,为进一步制定改善上海市大气环境质量的具体措施提出相关的参考建议,本文在查阅大量文献资料基础上,总结了上海市自2000年至2007年共8年大气环境质量现状分析,统计分析了主要污染物的变化特征,通过对相关环保措施、政府政策等方面资料的引用和分析,讨论了上海市大气环境质量变化的影响因素。分析结果表明:上海市连续三轮的"环保三年行动计划"的实施使上海市大气环境质量逐渐好转,大气污染情况逐步减轻,但由于产业结构调整带来的大气环境压力以及社会快速发展的压力,使得上海市治理大气环境污染的任务仍然艰巨。酸雨已经成为上海市大气环境的突出重要问题。     

中国煤炭消费对PM2.5污染的影响研究

国务院颁布的《大气污染防治行动计划》明确提出制定国家煤炭消费总量中长期控制目标,到2017年,煤炭占能源消费总量比重降低到65%以下,然而煤炭消费对PM_(2.5)污染的贡献到底多大,这是当前亟待研究的科学问题。为定量分析煤炭消费对我国PM_(2.5)污染的影响,本研究首先计算了2012年煤炭消费产生的大气污染物排量,然后利用CAMx空气质量模型,分别采用组分分析法和情景模拟法两种方法研究了煤炭消费对全国PM_(2.5)污染的影响。组分分析法研究表明,煤炭消费对全国PM_(2.5)年均浓度的贡献率约为61%,其中煤炭直接燃烧、煤炭相关行业的贡献率分别约为37%、24%;情景模拟法研究表明,煤炭消费对全国PM_(2.5)年均浓度的贡献率约为56%。因此,我国由于煤炭消费对全国PM_(2.5)年均浓度的贡献率为56%~61%。     

大气环境约束下的中国煤炭消费总量控制研究

煤炭消费过程中排放的大气污染物已成为我国大气污染的重要来源。本文采用WRF-CAMx 空气质量模型定量分析了煤炭消费- 污染物排放- 空气质量之间的影响关系,基于情景分析方法,研究了2020 年、2030年空气质量改善需求对地区大气污染物排放总量与煤炭消费总量的约束作用。在此基础上,结合重点地区行业发展与能源供需等因素,提出各省煤炭消费总量控制目标与控煤对策建议。研究结果表明,要实现2020 年、2030 年空气质量改善阶段性目标,全国煤炭消费总量应分别控制在40.8 亿吨和37.7 亿吨左右,京津冀鲁豫等11 个重点省份2020 年煤炭消费量应控制在15.8 亿吨、2030 年控制在13.1 亿吨,全国煤炭清洁化利用水平需要在当前基础上大幅度提升。     

环境质量管理新模式:启程与挑战

污染物总量控制是我国近10年环境保护中一个重要的治理模式。但在环境容量"硬约束"、公众对良好环境质量"硬需求"的大背景下,我国的环境管理应逐步从总量控制转向以环境质量改善为核心,改善环境质量已经成为环保工作的出发点和落脚点。2015年,随着新《环境保护法》的实施和"三大战役"的先后打响,法律保障、行动计划、政府问责、质量监测等逐步就绪,环境质量管理的基础手段不断夯实。2016年,环境质量管理新模式将全面启动,建议从强化公众环境健康、实行区域流域总量控制、改革生态环保管理体制、强化市场机制、推行排污许可证制度、加强信息公开和公众参与等方面着手,全面推进环境质量管理转型与创新。     

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     

国家“十四五”环境经济政策改革路线图

"十三五"时期环境经济政策对建立我国生态文明建设长效机制发挥了重要作用,"十四五"时期需要通过进一步深化环境经济政策改革与创新以适应新时代生态文明建设需要。本文研究提出了我国"十四五"时期环境经济政策改革思路、框架与重点,认为我国"十四五"时期环境经济政策改革要深入贯彻习近平生态文明思想,系统考虑政策改革创新面临的新形势和新要求,推进建立"两山"转化和环境质量达标的长效激励机制,突出环境质量持续改善激励、突出经济过程全链条调控,突出政策手段的系统优化与协同增效,突出政策执行能力保障。继续推进生态环境财政制度改革,深化绿色价格税费机制创新,推进建立多元化、市场化生态补偿制度,健全生态环境权益交易机制,完善绿色金融体系,并同步推进完善生态环境价值核算、环境信息公开和信用体系、资源环境名录、政策绩效评估等政策实施配套能力建设,构建全面支撑生态文明建设的环境经济政策体系,推进环境治理体系和治理能力现代化。     

国家海洋生态环境保护“十四五”战略路线图分析

2018年,国家海洋生态环境管理体制重组,为系统推进海洋生态环境质量改善奠定了基础。本文基于美丽中国建设的战略目标,在分析海洋生态环境保护现状、问题以及形势的基础上,提出坚持陆海统筹、区域联动、分区防控和精准治理的原则,建议协同推进"污染防治、生态修复、风险防范、能力建设、国际合作"五大领域任务,重点建设"法律规范、空间管控、标准规范、目标责任、许可管理"五大体系,最终实现"十四五"国家海洋生态环境保护目标。     

“十四五”时期生态环境保护重点方向和任务研究

立足于我国生态环境保护工作的现实形势和发展趋势,本文判断在"十四五"时期我国生态环境保护将走出环境库兹涅茨曲线峰值期,但继续提升生态环境质量的边际成本会上升。此外,"十四五"时期也将是生态环境保护的主次要矛盾转化期、经济社会发展和生态环境保护的阶段性和区域性分异并存期。基于此,立足于我国社会主义现代化强国新征程和实施"两步走"战略的总体部署,进一步贯彻习近平生态文明思想,本文提出了"十四五"时期我国生态环境保护工作的主线和原则,以及加快推进生态环境治理体系现代化进程的路径和重大工程,以期推动生态文明建设迈向新时代。     

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.     

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.     

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).     

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%.     

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).     

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.     

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.     

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.     

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.