Emission control

排放控制
  • 文章类型: Journal Article
    一种有前途的污染控制技术是冷等离子体驱动的化学处理。等离子体是在接近大气压-温度的反应器内的脉冲电气体放电。该系统由非常短的高压脉冲的连续流供电。待处理的废气流过反应器。应用的方法涉及开发强大的冷等离子体系统,工业应用和测量技术。在许多工业现场进行了系统测试,涉及控制空气中的VOC(挥发性有机化合物)和气味。电气,用最先进的方法收集化学和气味测量数据。为了解释测试数据,开发了脉冲等离子体化学的整体反应动力学的近似解。它涉及到兰伯特函数,为方便起见,一个简单的近似。后者表明,去除量,在很好的近似中,是单个变量的函数。该变量是电等离子体功率除以气流除以输入浓度。在结果部分中,我们表明,在某些情况下,可以在可接受的能量需求下去除高达99%的挥发性污染。在最后部分中,我们将通过实施(亚)纳秒脉冲等离子体和固态高压技术以及与催化剂技术的集成来探讨未来的效率提高。
    A promising pollution control technology is cold plasma driven chemical processing. The plasma is a pulsed electric gas discharge inside a near atmospheric-pressure-temperature reactor. The system is energized by a continuous stream of very short high-voltage pulses. The exhaust gas to be treated flows through the reactor. The methods applied involve the development of robust cold plasma systems, industrial applications and measuring technologies. Tests of the systems were performed at many industrial sites and involved control of airborne VOC (volatile organic compound) and odor. Electrical, chemical and odor measuring data were collected with state-of-the-art methods. To explain the test data an approximate solution of global reaction kinetics of pulsed plasma chemistry was developed. It involves the Lambert function and, for convenience, a simple approximation of it. The latter shows that the amount of removal, in good approximation, is a function of a single variable. This variable is electric plasma power divided by gas flow divided by input concentration. In the results sections we show that in some cases up to 99% of volatile pollution can be removed at an acceptable energy requirement. In the final sections we look into future efficiency enhancements by implementation of (sub)nanosecond pulsed plasma and solid state high-voltage technology and by integration with catalyst technology.
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  • 文章类型: Journal Article
    了解亚硝酸(HONO)的生产对于光化学研究至关重要,尤其是在像中国东部这样的污染环境中。在2018年春季臭氧光化学和中国出口实验(OPECE)期间,在农村沿海地区进行了气体和颗粒成分的原位测量。该数据集用于研究通过白天异质HONO生产的反应性氮的再循环。尽管农业燃烧期间HONO水平增加,对观测数据的分析并没有表明农业燃烧气溶胶比其他人为气溶胶更有效地生产HONO。Box和一维建模分析揭示了二氧化氮(NO2)之间的内在关系,颗粒硝酸盐(pNO3),和硝酸(HNO3),导致观察到的和模拟的HONO浓度与三种异质HONO产生机制中的任何一种之间具有可比的一致性,气溶胶上的光敏化NO2转化,pNO3的光解和HNO3的转化。这一发现强调了白天异质HONO生产途径的机理理解和定量参数化的不确定性。此外,对活性氮回收的影响,臭氧(O3)生产,和O3控制策略根据HONO生产机制的不同而有很大差异。在区域范围内,从pNO3中转化HONO可以大大提高O3的产量,而从NO2的转化可以降低受污染的中国东部地区O3对NOx变化的敏感性。
    Understanding of nitrous acid (HONO) production is crucial to photochemical studies, especially in polluted environments like eastern China. In-situ measurements of gaseous and particulate compositions were conducted at a rural coastal site during the 2018 spring Ozone Photochemistry and Export from China Experiment (OPECE). This data set was applied to investigate the recycling of reactive nitrogen through daytime heterogeneous HONO production. Although HONO levels increase during agricultural burning, analysis of the observation data does not indicate more efficient HONO production by agricultural burning aerosols than other anthropogenic aerosols. Box and 1-D modeling analyses reveal the intrinsic relationships between nitrogen dioxide (NO2), particulate nitrate (pNO3), and nitric acid (HNO3), resulting in comparable agreement between observed and simulated HONO concentrations with any one of the three heterogeneous HONO production mechanisms, photosensitized NO2 conversion on aerosols, photolysis of pNO3, and conversion from HNO3. This finding underscores the uncertainties in the mechanistic understanding and quantitative parametrizations of daytime heterogeneous HONO production pathways. Furthermore, the implications for reactive nitrogen recycling, ozone (O3) production, and O3 control strategies vary greatly depending on the HONO production mechanism. On a regional scale, the conversion of HONO from pNO3 can drastically enhance O3 production, while the conversion from NO2 can reduce O3 sensitivity to NOx changes in polluted eastern China.
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  • 文章类型: Journal Article
    荧光芳族脲化合物在乙酸根阴离子存在下经历激发态分子间质子转移(ESPT),以从配合物(N*)的激发态产生互变异构体(T*)的激发态,产生双重荧光。在这里,我们对带有取代基的蒽醌-1-基-3-苯基脲衍生物进行了光谱测量,-CF3,-F,或-Cl,在乙酸盐存在下,在苯基的对位上研究取代基对ESPT反应的影响以及N*和T*的失活过程。动力学分析表明,反向ESPT速率常数(k-PT)取决于各自的取代基,这表明每个取代基可能对反向ESPT过程的影响不同。特别是,由于-F的吸电子性质是通过-I和+Iπ效应估计的,-F具有轻微的供电子特性,并在激发态下影响从T*到N*的反向过程。这项研究表明,可以通过选择ESPT系统中的特定取代基来控制排放。
    Fluorescent aromatic urea compounds undergo excited-state intermolecular proton transfer (ESPT) in the presence of acetate anions to produce an excited state of the tautomer (T*) from the excited state of the complex (N*), resulting in dual fluorescence. Herein, we performed spectroscopic measurements of anthracen-1-yl-3-phenylurea derivatives with substituents, -CF3, -F, or -Cl, at the p-position of the phenyl group in the presence of acetate to investigate the substituent effects on the ESPT reaction and the deactivation processes of N* and T*. Kinetic analysis showed that the reverse ESPT rate constant (k-PT) depended on the respective substituents, suggesting that each substituent may influence the reverse ESPT process differently. In particular, since the electron-withdrawing properties of -F are estimated by the - I and + Iπ effects, it is plausible that -F has a slight electron-donating property and influences the reverse process from T* to N* in the excited state. This study shows that it is possible to control emission by selecting specific substituents in the ESPT system.
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  • 文章类型: Journal Article
    中国人为活动导致的高活性氮(N)排放导致氮沉降增加和生态系统退化。自2010年以来,中国政府严格管制反应性氮排放,确定N沉积是否减少需要长期监测。这里,我们报告了过去十年来中国东北农村森林遗址(清远)的氮沉积模式。我们收集了2014年至2022年的456个日降水样本,并分析了氮沉积的时间动态。NH4+-N,NO3--N,总无机氮(TIN)沉积范围为10.5±3.5(平均值±SD),6.1±1.6和16.6±4.7kgNha-1年-1。在测量期间,清远的锡沉积减少了55%,而东亚可比地区的这一数字下降了14-34%。我们使用随机森林模型来确定影响NH4-N沉积的因素,NO3--N,和TIN在研究期间。由于农业NH3排放量的减少,NH4-N沉积减少了60%。此外,NO3--N沉积减少42%,由于减少了农业土壤和化石燃料燃烧的NOx排放。中国东北地区氮沉积的急剧下降归因于煤炭消耗的减少,改进汽车排放控制,以及农业实践的转变。需要进行长期监测,以评估区域空气质量和N排放控制法规的影响。
    High reactive nitrogen (N) emissions due to anthropogenic activities in China have led to an increase in N deposition and ecosystem degradation. The Chinese government has strictly regulated reactive N emissions since 2010, however, determining whether N deposition has reduced requires long-term monitoring. Here, we report the patterns of N deposition at a rural forest site (Qingyuan) in northeastern China over the last decade. We collected 456 daily precipitation samples from 2014 to 2022 and analysed the temporal dynamics of N deposition. NH4+-N, NO3--N, and total inorganic N (TIN) deposition ranged from 10.5 ± 3.5 (mean ± SD), 6.1 ± 1.6, and 16.6 ± 4.7 kg N ha-1 year-1, respectively. Over the measurement period, TIN deposition at Qingyuan decreased by 55 %, whereas that in comparable sites in East Asia declined by 14-34 %. We used a random forest model to determine factors influencing the deposition of NH4+-N, NO3--N, and TIN during the study period. NH4+-N deposition decreased by 60 % because of decreased agricultural NH3 emissions. Furthermore, NO3--N deposition decreased by 42 %, due to reduced NOx emissions from agricultural soil and fossil fuel combustion. The steep decline in N deposition in northeastern China was attributed to reduced coal consumption, improved emission controls on automobiles, and shifts in agricultural practices. Long-term monitoring is needed to assess regional air quality and the impact of N emission control regulations.
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  • 文章类型: Journal Article
    煤炭燃烧是全球有毒硒(Se)排放的主要原因。煤中的无机元素显着影响燃烧过程中的硒分配。这项工作证实,与其他主要元素相比,灰分中的钙(Ca)与1300°C下的Se保留具有更强的关系。Ca氧化物与气态Se发生化学反应,在300-1300°C下,其烧结致密化对Se吸附能力(44.45-1840.71→35.17-1540.15mg/kg)的影响很小。因此,煤中的Ca被确定为具有阻碍气态Se排放的潜力,在350MW机组中使用了Ca含量增加的煤(2.74→5.19wt%)。空气预热器入口(320-362°C)烟气中Se质量分布的降低(3.54%→2.63%)证实了Ca含量增加对减少气态Se排放的有效性。更多的气态Se进一步冷凝,并在通过静电除尘器时被粉煤灰化学吸附,导致粉煤灰中Se含量显著增加。此外,相应的硒浸出率从4.88-35.74%下降到1.87-26.31%,表明粉煤灰中富硒的稳定性增强。这项研究证实了通过增加煤中的Ca含量将烟气中的气态硒固存到粉煤灰中的可行性和环境安全性。
    Coal combustion is the major contributor to global toxic selenium (Se) emissions. Inorganic elements in coals significantly affect Se partitioning during combustion. This work confirmed that the calcium (Ca) in ash had a stronger relationship with Se retention at 1300 °C than other major elements. Ca oxide chemically reacted with gaseous Se, and its sintering densification slightly affected Se adsorption capacities (44.45 -1840.71→35.17 -1540.15 mg/kg) at 300 - 1300 °C. Therefore, Ca in coals was identified as having potential for hindering gaseous Se emissions, and coals with increased Ca contents (2.74→5.19 wt%) were used in a 350 MW unit. The decreased Se mass distribution (3.54%→2.63%) in flue gas at air preheater inlet (320 -362 °C) confirmed the effectiveness of increased Ca content on gaseous Se emission reduction. More gaseous Se further condensed and was chemically adsorbed by fly ash when passed through an electrostatic precipitator, resulting in a significant increase in the Se content of fly ash. Additionally, the corresponding Se leaching ratio decreased from 4.88 - 35.74% to 1.87 - 26.31%, indicating enhanced stability of Se enriched in fly ash. This research confirmed the feasibility and environmental safety of sequestration of gaseous Se from flue gas to fly ash by increasing the Ca content in coals.
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  • 文章类型: Systematic Review
    燃煤发电厂(CFPP)是《水50%公约》认证的最重要的汞排放源之一,近年来备受关注。在这项研究中,我们使用WebofScience和CiteSpace分析了2000年至2022年该领域的知识结构,然后对其进行了系统的回顾。燃煤电厂汞排放领域稳步发展。研究热点可分为三类:(1)以形态变化和排放计算为重点的排放表征研究;(2)以控制技术为重点的排放控制研究;(3)以环境污染和健康风险为重点的环境影响研究。总之,使用富氧气氛进行燃烧并安装高效空气污染控制装置(APCD)有助于减少Hg0的形成。超低排放改造后的APCD和改性吸附剂的平均汞去除率分布在82-93%和41-100%之间。分别。脱硫污泥中燃烧副产物汞的风险水平最高(RAC>10%),其次是粉煤灰(10% Coal-fired power plants (CFPPs) are one of the most significant sources of mercury (Hg) emissions certified by the Minamata Convention, which has attracted much attention in recent years. In this study, we used the Web of Science and CiteSpace to analyze the knowledge structure of this field from 2000 to 2022 and then reviewed it systematically. The field of Hg emissions from coal-fired power plants has developed steadily. The research hotspots can be divided into three categories: (1) emission characterization research focused on speciation changes and emission calculations; (2) emission control research focused on control technologies; (3) environmental impact research focused on environmental pollution and health risk. In conclusion, using an oxygen-rich atmosphere for combustion and installing high-efficiency air pollution control devices (APCDs) helped to reduce the formation of Hg0. The average Hg removal rates of APCDs and modified adsorbents after ultra-low emission retrofit were distributed in the range of 82-93% and 41-100%, respectively. The risk level of Hg in combustion by-products was highest in desulfurization sludge (RAC > 10%) followed by fly ash (10% < RAC < 30%) and desulfurization gypsum (1% < RAC < 10%). Additionally, we found that the implementation of pollution and carbon reduction policies in China had reduced Hg emissions from CFPPs by 45% from 2007 to 2015, increased the efficiency of Hg removal from APCDs to a maximum of 96%, and reduced global transport and health risk of atmospheric Hg. The results conjunctively achieved by CiteSpace, and the literature review will enhance understanding of CFPP Hg emission research and provide new perspectives for future research.
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  • 文章类型: Journal Article
    感知器模型已成为工程领域模式识别和分类问题的重要工具。这项研究设想实施人工神经网络来预测用于脱硫活动的微型喷雾干燥器的性能。这项工作采用了k折交叉验证,评估跨多个数据段的模型性能的严格技术。几个ANN模型(21)在从硫酸化条件获得的数据上进行了训练,包括硫酸化温度(120°C-200°C),浆液pH值(4-12),化学计量比(0.5-2.5),浆料固体浓度(6%-14%)作为进料输入和硫捕获作为响应。在logsig和tansig激活函数触发的神经网络上进行仿真之前,使用高斯噪声数据增强生成的三百个合成数据集经历了10倍交叉验证过程。通过将隐藏单元的数量从2更改为10来进一步评估计算精度。使用统计指标,如均方误差(MSE),均方根误差(RMSE),平均绝对百分比误差(MAPE),和决定系数(R2)技术。总的来说,误差估计表明,交叉验证和数据增强在有效的神经网络泛化中至关重要。当映射到实际值时,用10个隐藏单元格训练的logsig函数呈现更紧密的数据衔接。
    Perceptron models have become integral tools for pattern recognition and classification problems in engineering fields. This study envisioned implementing artificial neural networks to forecast the performance of a mini-spray dryer for desulfurization activities. This work adopted k-fold cross-validation, a rigorous technique that evaluates model performance across multiple data segments. Several ANN models (21) were trained on data obtained from sulfation conditions, including sulfation temperature (120 °C-200 °C), slurry pH (4-12), stoichiometric ratio (0.5-2.5), slurry solid concentration (6%-14%) as the feed input and sulfur capture as the response. Three hundred synthetic datasets generated using the Gaussian noise data augmentation underwent a 10-fold cross-validation process before simulation on neural networks triggered by the logsig and tansig activation functions. The computation accuracy was further evaluated by altering the number of hidden cells from 2 to 10. The ANN architectures were assessed using statistical metrics such as mean square error (MSE), root mean square error (RMSE), mean absolute percentage error (MAPE), and the coefficient of determination (R2) techniques. Overall, error estimation suggests cross-validation and data augmentation are critical in efficient neural network generalization. The logsig function trained with 10 hidden cells presented closer data articulation when mapped onto actual values.
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  • 文章类型: Journal Article
    要确定优先级控制源,提出了一种方法来评估吸入PM2.5结合重金属(PBHM)对健康风险的来源特异性贡献.从北京市区和郊区共采集了482个每日PM2.5样本,中国,在2018年至2019年之间。除了PMF-PSCF模型,建立了Pb同位素同源源模型,以实现更可靠的源解析。通过使用残疾调整寿命年(DALYs)的综合指标,可以在统一的尺度上比较致癌和非致癌的健康风险。研究发现,市郊地区总PBHM的年平均浓度明显高于市区,在供暖季节的浓度明显高于非供暖季节。综合粉尘对PBHM的浓度贡献最大,whilecoalburnitioncontributedthemosttotheDALYsassociatedwithPBHM.TheseresultssuggeststhatprioritizingthecontrolofcoalburnitioncouldeffectivelyreducethediseasyburtassociatedwithPBHM,带来显著的公共卫生益处。
    To determine the priority control sources, an approach was proposed to evaluate the source-specific contribution to health risks from inhaling PM2.5-bound heavy metals (PBHMs). A total of 482 daily PM2.5 samples were collected from urban and suburban areas of Beijing, China, between 2018 and 2019. In addition to the PMF-PSCF model, a Pb isotopic IsoSource model was built for more reliable source apportionment. By using the comprehensive indicator of disability-adjusted life years (DALYs), carcinogenic and noncarcinogenic health risks could be compared on a unified scale. The study found that the annual average concentrations of the total PBHMs were significantly higher in suburban areas than in urban areas, with significantly higher concentrations during the heating season than during the nonheating season. Comprehensive dust accounted for the largest contribution to the concentration of PBHMs, while coal combustion contributed the most to the DALYs associated with PBHMs. These results suggest that prioritizing the control of coal combustion could effectively reduce the disease burden associated with PBHMs, leading to notable public health benefits.
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  • 文章类型: Journal Article
    通过整合工业生产,使用多目标规划构建了中国实现碳中和的低成本路径系统,电力,加热,交通运输,和森林碳固存。我们的目标是最大限度地降低系统的总成本,二氧化碳排放,和空气污染物。这些制约因素包括中国在2030年之前达到二氧化碳排放峰值的目标;在2060年之前实现碳中和;确保工业,电源,加热,和运输用品;推广绿色能源;实施排放控制。该模型占煤炭消耗高的行业,如钢铁和化学工业。考虑了各种电源,包括燃煤,核,风,和太阳能。采用森林碳汇和碳捕获与封存技术来实现减排目标。模型,使用现有的研究数据进行了验证,提供了具有成本效益的路径方案,并表现出很高的有效性。我们的发现强调了结构调整和排放控制的重要性,用电力,加热,和运输部门比其他行业表现出更高的可行性,并为实现碳中和提供更大的贡献。相反,钢铁等行业的产业转型,化学,建筑材料的可行性低,贡献有限。建模结果为开发低成本,中国复杂系统中的碳排放目标运输结构。此处提供的结果表明,该方法在促进旨在实现关键碳减排目标的计划方面具有全球适用性。
    A low-cost path system for achieving carbon neutrality in China was modelled using multi-objective programming by integrating industrial production, electric power, heating, transportation, and forest carbon sequestration. We aimed to minimise the total system cost, CO2 emissions, and air pollutants. The constraints included China\'s targets of peaking CO2 emissions before 2030; achieving carbon neutrality before 2060; ensuring industry, power, heating, and transportation supplies; promoting green energy; and implementing emission control. The model accounted for industries with high coal consumption, such as steel and chemical industries. Various power sources were considered, including coal-fired, nuclear, wind, and solar energy. Forest carbon sink and carbon capture and storage technologies were employed to achieve the emission reduction goals. The model, which was validated using available research data, offered cost-effective path schemes and exhibited high validity. Our findings emphasise the importance of structural adjustments and emission control, with electric power, heating, and transportation sectors showing higher feasibility and providing greater contributions to achieving carbon neutrality than other industries. Conversely, industrial transformation in sectors such as iron and steel, chemical, and construction materials had low feasibility and limited contribution. The modelling outcomes provide valuable insights for developing low-cost, carbon emission-targeted transportation structures in China\'s complex system. The results presented here demonstrate the global applicability of this method in contributing to plans aimed at meeting key carbon reduction targets.
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  • 文章类型: Journal Article
    化学工业是非甲烷挥发性有机化合物(NMVOCs)的重要来源,环境臭氧(O3)的关键前体,和次级有机气溶胶(SOA)。尽管它们很重要,对这些排放的精确估计仍然具有挑战性,阻碍NMVOC控制的实施。这里,我们首次对中国化学工业的NMVOC排放进行了全面的工厂级评估,涵盖3461种植物,127个产品,2010年至2019年有50种NMVOC化合物。我们的研究结果表明,2019年中国化工行业总共排放了3105Gg(四分位数范围:1179-8113)NMVOCs,其中一些特定产品占排放量的大部分。一般来说,从事化学纤维生产或位于中国东部的工厂,由于O3和SOA的形成潜力较高或靠近居民区或两者兼而有之,对公众健康构成更大的风险。我们证明,与目前的情况相比,以这些高风险植物为目标进行减排,平均每单位减排可将健康益处提高7-37%。因此,本研究为在中国化学工业中制定有效的植物特异性NMVOC控制策略提供了重要的见解。
    The chemical industry is a significant source of nonmethane volatile organic compounds (NMVOCs), pivotal precursors to ambient ozone (O3), and secondary organic aerosol (SOA). Despite their importance, precise estimation of these emissions remains challenging, impeding the implementation of NMVOC controls. Here, we present the first comprehensive plant-level assessment of NMVOC emissions from the chemical industry in China, encompassing 3461 plants, 127 products, and 50 NMVOC compounds from 2010 to 2019. Our findings revealed that the chemical industry in China emitted a total of 3105 (interquartile range: 1179-8113) Gg of NMVOCs in 2019, with a few specific products accounting for the majority of the emissions. Generally, plants engaged in chemical fibers production or situated in eastern China pose a greater risk to public health due to their higher formation potentials of O3 and SOA or their proximity to residential areas or both. We demonstrated that targeting these high-risk plants for emission reduction could enhance health benefits by 7-37% per unit of emission reduction on average compared to the current situation. Consequently, this study provides essential insights for developing effective plant-specific NMVOC control strategies within China\'s chemical industry.
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