reactive nitrogen

活性氮
  • 文章类型: Journal Article
    作为两种重要的环境空气污染物,颗粒物(PM2.5)和臭氧(O3)都可能来自气体氮氧化物。在这项研究中,通过理论分析和机器学习方法,我们研究了大气活性氮对PM2.5-O3污染的影响,其中一氧化氮(NO),二氧化氮(NO2),气态硝酸(HNO3)和颗粒硝酸盐(pNO3-)转化过程对PM2.5-O3污染具有共向和反向作用。其中,HNO3和SO2是导致PM2.5和O3同时增长或降低的同向驱动因子;而NO,NO2和温度代表反向因素,可以促进一种污染物的生长,减少另一种污染物的生长。我们的发现表明,为可持续减少PM2.5-O3设计合适的共同控制策略应通过考虑在合适的敏感区域下的反方向和同方向效应来针对驱动因素。对于同向驱动因素,设计合适的缓解策略将共同实现PM2.5和O3的有效减少;而对于反向驱动因素,它应该更有耐心,否则,可以减少一项,但同时增加另一项。
    As the two important ambient air pollutants, particulate matter (PM2.5) and ozone (O3) can both originate from gas nitrogen oxides. In this study, applied by theoretical analysis and machine learning method, we examined the effects of atmospheric reactive nitrogen on PM2.5-O3 pollution, in which nitric oxide (NO), nitrogen dioxide (NO2), gaseous nitric acid (HNO3) and particle nitrate (pNO3-) conversion process has the co-directional and contra-directional effects on PM2.5-O3 pollution. Of which, HNO3 and SO2 are the co-directional driving factors resulting in PM2.5 and O3 growing or decreasing simultaneously; while NO, NO2, and temperature represent the contra-directional factors, which can promote the growth of one pollutant and reduce another one. Our findings suggest that designing the suitable co-controlling strategies for PM2.5-O3 sustainable reduction should target at driving factors by considering the contra-directional and co-directional effects under suitable sensitivity regions. For co-directional driving factors, the design of suitable mitigation strategies will jointly achieve effective reduction in PM2.5 and O3; while for contra-directional driving factors, it should be more patient, otherwise, it is possible to reduce one item but increase another one at the same time.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    氮氧化物(NOx)应根据环境法规进行净化,逐年受到限制。各种各样的脱硝技术,例如通过注入还原剂如氨(NH3)将NOx选择性催化还原(SCR)为氮气(N2)和将NOx存储还原(NSR)为N2,到目前为止,已经在实践中得到了发展。复杂的催化方法对于能源的可持续性(包括NOx的完全净化)可能是强制性的。作为同时克服环境和资源问题的解决方案之一,这篇概念文章重点介绍了活性氮(Nr)化合物的利用,主要是NOx,鼓励开放考虑氮循环经济。对于经由NH3的NOx的再循环,可以通过在不改变反应温度的操作的情况下在含NOx的氧化气体和含H2的还原性气体之间交替地切换入口气体来提出具有挑战性但合理的催化技术。考虑到NOx的反应性高于N2的反应性,这种NOx至NH3(NTA)工艺有望用于NH3合成,不仅作为肥料而且在不久的将来作为燃料都很有价值。
    Nitrogen oxides (NOx) should be purified according to environmental regulations, being restricted increasingly year by year. A wide variety of denitration technologies, such as selective catalytic reduction (SCR) of NOx to nitrogen (N2) and NOx storage reduction (NSR) to N2 by injecting reducing agents like ammonia (NH3), has so far been developed practically. Sophisticated catalytic approaches are perhaps mandatory for the sustainability in energy including complete purification of NOx. As one of the solutions to overcome problems for environment and resource simultaneously, this concept article focuses on the utilization of reactive nitrogen (Nr) compounds, mainly NOx, for encouraging an opening to consider nitrogen circular economy. For the recycling of NOx via NH3, a challenging but rational catalytic technology can be proposed by an alternate switching the inlet gas between NOx containing oxidative gas and H2 containing reductive one without an operation to change the reaction temperature. Considering the reactivity of NOx higher than that of N2, this kind of NOx to NH3 (NTA) process is promising for synthesizing NH3, being valuable not only as fertilizer but also as fuel in near future.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    饮食营养操作(例如蛋白质部分)可以降低反刍动物的环境足迹,特别是活性氮(N)。本研究调查了日粮可溶性蛋白(SP)水平降低的粗蛋白质(CP)对肠氮吸收的影响。后肠氮代谢,粪便微生物群和代谢物,以及它们与N代谢表型的联系。32只雄性胡羊,年龄为6个月,初始体重为40.37±1.18公斤,被随机分配到四个饮食组。控制饮食(CON),符合NRC标准,以干物质为基础保持16.7%的CP含量。相反,实验饮食(LPA,LPB,和LPC)与CON相比,CP降低了10%,伴随着SP调整到21.2%,25.9%,和29.4%的CP,分别。我们的结果表明,低蛋白饮食导致血浆肌酐浓度显着降低,氨,尿素N,粪便总短链脂肪酸(SCFA)(P<0.05)。值得注意的是,与LPA相比,LPB和LPC表现出增加的总SCFA和丙酸浓度(P<0.05)。与能量代谢和氨基酸(AA)生物合成途径相关的粪便微生物群中Prevotella属的富集明显,低蛋白饮食中的SP水平约为25%至30%。此外,LPB和LPC日粮显示粪便NH4-N和NO2--N含量以及脲酶活性降低,与CON相比(P<0.05)。同时,粪便谷氨酸脱氢酶基因(gdh)的减少,亚硝酸还原酶基因(nirS),观察到一氧化氮还原酶基因(norB)丰度(P<0.05),指向源头反应性氮产量的潜在减少。意义重大,小肠中AA和肽转运蛋白的mRNA丰度上调(十二指肠,空肠,和回肠)和血浆AA浓度升高(例如精氨酸,蛋氨酸,天冬氨酸,谷氨酸,等。)强调了氮吸收和氮效率的增强。总之,CP减少10%,再加上大约25%到30%的SP水平,证明了通过粪便Prevotella富集减少反应性N排放并提高肠道能量和N利用效率的潜力。
    Dietary nutrient manipulation (e.g. protein fractions) could lower the environmental footprints of ruminants, especially reactive nitrogen (N). This study investigated the impacts of dietary soluble protein (SP) levels with decreased crude protein (CP) on intestinal N absorption, hindgut N metabolism, fecal microbiota and metabolites, and their linkage with N metabolism phenotype. Thirty-two male Hu sheep, with an age of six months and an initial BW of 40.37 ± 1.18 kg, were randomly assigned to four dietary groups. The control diet (CON), aligning with NRC standards, maintained a CP content of 16.7% on a dry matter basis. Conversely, the experimental diets (LPA, LPB, and LPC) featured a 10% reduction in CP compared with CON, accompanied by SP adjustments to 21.2%, 25.9%, and 29.4% of CP, respectively. Our results showed that low-protein diets led to significant reductions in the concentrations of plasma creatinine, ammonia, urea N, and fecal total short-chain fatty acids (SCFA) (P < 0.05). Notably, LPB and LPC exhibited increased total SCFA and propionate concentrations compared with LPA (P < 0.05). The enrichment of the Prevotella genus in fecal microbiota associated with energy metabolism and amino acid (AA) biosynthesis pathways was evident with SP levels in low-protein diets of approximately 25% to 30%. Moreover, LPB and LPC diets demonstrated a decrease in fecal NH 4 + -N and NO 2 - -N contents as well as urease activity, compared with CON (P < 0.05). Concomitantly, reductions in fecal glutamic acid dehydrogenase gene (gdh), nitrite reductase gene (nirS), and nitric oxide reductase gene (norB) abundances were observed (P < 0.05), pointing towards a potential reduction in reactive N production at the source. Of significance, the up-regulation of mRNA abundance of AA and peptide transporters in the small intestine (duodenum, jejunum, and ileum) and the elevated concentration of plasma AA (e.g. arginine, methionine, aspartate, glutamate, etc.) underscored the enhancement of N absorption and N efficiency. In summary, a 10% reduction in CP, coupled with an SP level of approximately 25% to 30%, demonstrated the potential to curtail reactive N emissions through fecal Prevotella enrichment and improve intestinal energy and N utilization efficiency.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

       PDF(Pubmed)

  • 文章类型: Journal Article
    大气硝酸盐,包括硝酸(HNO3),颗粒硝酸盐(pNO3),和有机硝酸盐(RONO2),是对空气质量有影响的关键大气成分,养分沉积,和气候。然而,在大气化学模型中准确表示大气硝酸盐浓度是一个持续的挑战。造成这一挑战的一个因素是涉及HNO3形成的复杂化学转化,模型很难复制。这里,我们提出了一种新颖的模型框架,该框架利用氧稳定同位素异常(Δ17O)来定量描述臭氧(O3)参与前体氮氧化物NOx=NONO2光化学循环和HNO3形成。该框架已集成到美国EPA社区多尺度空气质量(CMAQ)建模系统中,以促进对NOx氧化和HNO3形成的全面评估。在美国东北部的应用中,模型Δ17O与最近进行的昼夜Δ17O(NO2)和时空Δ17O(HNO3)观测结果比较好,对于Δ17O(HNO3),模型与观测值之间的均方根误差为2.6‰。该模型表明,美国东北部每年产生HNO3的主要形成途径是NOOH(46%),N2O5水解(34%),和有机硝酸盐水解(12%)。该模型可以在未来涉及活性氮的空气质量和沉积研究中评估CMAQ中的NOx化学。
    Atmospheric nitrate, including nitric acid (HNO3), particulate nitrate (pNO3), and organic nitrate (RONO2), is a key atmosphere component with implications for air quality, nutrient deposition, and climate. However, accurately representing atmospheric nitrate concentrations within atmospheric chemistry models is a persistent challenge. A contributing factor to this challenge is the intricate chemical transformations involving HNO3 formation, which can be difficult for models to replicate. Here, we present a novel model framework that utilizes the oxygen stable isotope anomaly (Δ17O) to quantitatively depict ozone (O3) involvement in precursor nitrogen oxides N O x = N O + N O 2 photochemical cycling and HNO3 formation. This framework has been integrated into the US EPA Community Multiscale Air Quality (CMAQ) modeling system to facilitate a comprehensive assessment of NO x oxidation and HNO3 formation. In application across the northeastern US, the model Δ17O compares well with recently conducted diurnal Δ17O(NO2) and spatiotemporal Δ17O(HNO3) observations, with a root mean square error between model and observations of 2.6 ‰ for Δ17O(HNO3). The model indicates the major formation pathways of annual HNO3 production within the northeastern US are NO+OH (46 %), N2O5 hydrolysis (34 %), and organic nitrate hydrolysis (12 %). This model can evaluate NO x chemistry in CMAQ in future air quality and deposition studies involving reactive nitrogen.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

       PDF(Pubmed)

  • 文章类型: Journal Article
    活性氧(ROS),活性硫物种(RSS),金属离子,和氮物种(RNS)在各种生物过程中发挥重要作用,比如信号转导,炎症,和神经退行性损伤。这些物种,虽然对于某些功能至关重要,也会诱发与压力有关的疾病。ROS之间的相互关系,RSS,金属离子和RNS强调了量化它们在活细胞中的浓度的重要性,组织,和有机体。该综述强调使用基于小分子的荧光/化学剂量计探针,以有效地测量和绘制物种分布,具有高时间和空间精度,特别注意体外和体内环境。这些探针被认为是有助于现代氧化还原生物学突破的有价值的工具。该评论专门讨论了HOCl/ClO(次氯酸/次氯酸盐)与其他反应性物种的关系。(双传感探头)。
    Reactive oxygen species (ROS), reactive sulfur species (RSS), metal ions, and nitrogen species (RNS) play important roles in a variety of biological processes, such as a signal transduction, inflammation, and neurodegenerative damage. These species, while essential for certain functions, can also induce stress-related diseases. The interrelation between ROS, RSS, Metal ions and RNS underscores the importance of quantifying their concentrations in live cells, tissues, and organisms. The review emphasizes the use of small-molecule-based fluorescent/chemodosimeter probes to effectively measure and map the species\' distribution with high temporal and spatial precision, paying particular attention to in vitro and in vivo environments. These probes are recognized as valuable tools contributing to breakthroughs in modern redox biology. The review specifically addresses the relationship of HOCl/ClO‾ (hypochlorous acid/Hypochlorite) with other reactive species. (Dual sensing probes).
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    氨(NH3)是大气中所有活性氮物种中的主要成分,和次级无机气溶胶形成的最重要物种。最近基于卫星的观测已将印度恒河平原(IGP)确定为全球NH3排放的主要热点;但是,对影响其丰度的主要来源和大气过程知之甚少。本研究旨在了解半城市地区冬季NH3的来源(Patiala,30.3°N,76.4°E,249mamsl)位于IGP中,使用PM2.5中的物种特异性δ15N。观察到总氮(δ15N-TN)和铵(δ15N-NH4)的稳定同位素特征的明显昼夜变化;尽管,TN和NH4+的平均昼夜浓度相似。使用δ15N-NH3的混合模型结果揭示了非农业排放(NH3泄漏:47±24%)相对于农业排放(24±11%)的优势。燃烧源(19±14%),和大气NH3的生物质燃烧(10±8%)。对NH3的源贡献的日变化微不足道。Further,观察到δ15N-NH4+与环境相对湿度(RH)和白天NO3--N浓度呈显著负相关,并归因于NH4NO3在白天挥发的可能性,由于较低的RH和较高的温度,导致气溶胶相中剩余的NH4同位素富集。这项研究,第一次来自印度,强调了非农业NH3排放在农业主导的IGP地区的重要性,以及局部气象学对气溶胶NH4中δ15N同位素分馏的作用。
    Ammonia (NH3) is the major constituent among all the reactive nitrogen species present in the atmosphere, and the most essential species for secondary inorganic aerosol formation. Recent satellite-based observations have identified the Indo-Gangetic Plain (IGP) as a major hotspot of global NH3 emission; however, the major sources and atmospheric processes affecting its abundance are poorly understood. The present study aims to understand the wintertime sources of NH3 over a semi-urban site (Patiala, 30.3°N, 76.4°E, 249 m amsl) located in the IGP using species specific δ15N in PM2.5. A distinct diurnal variation in the stable isotopic signature of total nitrogen (δ15N-TN) and ammonium (δ15N-NH4+) were observed; although, average day and night time concentrations of TN and NH4+ were similar. Mixing model results using δ15N-NH3 reveal the dominance of non-agricultural emissions (NH3 slip: 47 ± 24%) over agricultural emissions (24 ± 11%), combustion sources (19 ± 14 %), and biomass burning (10 ± 8%) for atmospheric NH3. Diurnal variability in source contributions to NH3 was insignificant. Further, significantly negative correlations of δ15N-NH4+ with ambient relative humidity (RH) and daytime NO3--N concentration were observed, and attributed to the possibility of NH4NO3 volatilization during day-time owing to lower RH and higher temperature, resulting in isotopic enrichment of the remaining NH4+ in aerosol phase. This study, a first of its type from India, highlights the importance of non-agricultural NH3 emissions over the agriculture dominated IGP region, and the role of local meteorology on the isotopic fractionation of δ15N in aerosol NH4+.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    人为的活性氮(Nr)损失一直是一个关键的环境问题。然而,由于数据可用性和适当方法的限制,在精细尺度上对稻田的Nr损失和相关空间格局的估计仍不清楚。这里,我们估计了背景Nr损失(BNL,即,未施肥土壤的Nr损失)和损失因子(合成肥料的Nr损失百分比,LFs)用于稻田中的五种损失途径,并使用数据驱动模型结合多源数据确定了全国1×1km的空间变化。基于建立的机器学习模型,平均23.4%(15.3-34.6%,95%置信区间)的合成氮肥流失到环境中,以NH3的形式(17.4%,10.9-26.7%),N2O(0.5%,0.3-0.8%),NO(0.2%,0.1-0.4%),N浸出(3.1%,0.8-5.7%),和径流(2.3%,0.6-4.5%)。2021年中国稻田的Nr总损失估计为1.92±0.52TgNyr-1,其中合成肥料引起的Nr损失占69%,BNL占其他31%。Nr流失的热点集中在长江中下游地区,广泛种植水稻的地区。这项研究提高了Nr损失的估计精度,并确定了热点,这可以为政策制定者提供最新的见解,以确定缓解NR损失的优先事项和战略。
    Anthropogenic reactive nitrogen (Nr) loss has been a critical environmental issue. However, due to the limitations of data availability and appropriate methods, the estimation of Nr loss from rice paddies and associated spatial patterns at a fine scale remain unclear. Here, we estimated the background Nr loss (BNL, i.e., Nr loss from soils without fertilization) and the loss factors (the percentage of Nr loss from synthetic fertilizer, LFs) for five loss pathways in rice paddies and identified the national 1 × 1 km spatial variations using data-driven models combined with multi-source data. Based on established machine learning models, an average of 23.4% (15.3-34.6%, 95% confidence interval) of the synthetic N fertilizer was lost to the environment, in the forms of NH3 (17.4%, 10.9-26.7%), N2O (0.5%, 0.3-0.8%), NO (0.2%, 0.1-0.4%), N leaching (3.1%, 0.8-5.7%), and runoff (2.3%, 0.6-4.5%). The total Nr loss from Chinese rice paddies was estimated to be 1.92 ± 0.52 Tg N yr-1 in 2021, in which synthetic fertilizer-induced Nr loss accounted for 69% and BNL accounted for the other 31%. The hotspots of Nr loss were concentrated in the middle and lower regions of the Yangtze River, an area with extensive rice cultivation. This study improved the estimation accuracy of Nr losses and identified the hotspots, which could provide updated insights for policymakers to set the priorities and strategies for Nr loss mitigation.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    奥地利反应性氮(Nr)损失到地表水中的数量和途径,土壤,和大气是在2041-2070年的四种气候变化情景下确定的。使用两种营养素模型在两种不同的尺度下进行分析。首先,半经验性的,为奥地利建立了概念模型(MONERIS)来计算年度净盈余,对Nr的流量进行分类,并确定Nr损失的区域热点。其次,在三个农业流域建立了基于物理的生态水文模型(SWAT),以确定与Nr运输相关的水文过程,并以详细的时空分辨率量化农田中各种途径的运输量。修订了奥地利的农业N盈余计算,并将其用作两个模型的输入数据。MONERIS和SWAT模拟的输送到水体中的无机氮负荷总体相似,地下无机氮负荷的平均差异为±3kgha-1yr-1,表面无机氮负荷的平均差异为0.4至-0.03kgha-1yr-1。未来气候情景下作物氮素损失取决于肥料类型,种植的作物及其积累的生物量,以及气候情景的类型(潮湿或干燥)。在SWAT模型中,对输入数据(气候数据和参数值)的敏感性进行的检查发现,对模拟每月排放量的敏感性的主要贡献来自气候数据(69%至98%)。对于模拟N个载荷,气候情景占敏感性的30%至89%。在气候情景下模拟Nr流量是评估N损失关键区域并确定未来N运输途径的相关政策。使用双模型方法节省了设置复杂、大规模的数据密集型模型,并且可以详细关注关键集水区。
    The amounts and pathways of reactive nitrogen (Nr) losses in Austria into the surface water, soil, and atmosphere were determined under four climate change scenarios for the period 2041-2070. Two nutrient models were used to undertake the analysis at two different scales. Firstly, a semi-empirical, conceptual model (MONERIS) was setup for Austria to calculate the overall annual Nr surpluses, categorise flows of Nr, and identify regional hotspots of Nr losses. Secondly, a physically based eco-hydrological model (SWAT) was setup in three agricultural catchments to determine the hydrological processes related to Nr transport and quantify the amounts transported by various pathways in cropland at a detailed spatial and temporal resolution. The agricultural N surplus calculations for Austria were revised and used as input data for both models. The MONERIS and SWAT simulated inorganic N loads transported into waterbodies are overall similar, with average differences for the subsurface inorganic N loads of ±3 kg ha-1 yr-1 and for surface inorganic N loads of +0.4 to -0.03 kg ha-1 yr-1. Crop level N losses under future climate scenarios was contingent upon the fertilizer type, the crop grown and its accumulated biomass, as well as the type of climate scenario (wet or dry). In the SWAT model, an examination of the sensitivity of the input data (climate data and parameter values) found the dominant contribution to the sensitivity of simulated monthly discharge was from the climate data (69 % to 98 %). For simulating N loads, the climate scenarios contributed 30 % to 89 % of the sensitivity. Simulating Nr flows under climate scenarios is policy relevant to assess critical areas of N losses and identify future N transport pathways. Using a dual-model approach saves on resources required to set up a complex, data intensive model at a large scale, and can focus on critical catchments in detail.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    长寿命的温室气体一氧化二氮(N2O)和短寿命的活性氮(Nr)气体,如氨(NH3),亚硝酸(HONO),和氮氧化物(NOx)从施肥的土壤中产生和排放,对气候变暖和空气质量起着至关重要的作用。然而,只有很少的研究同时量化了农业土壤中长期和短期气态氮(N)物种的生产和排放潜力。为了将气态N物种与中间N化合物[铵(NH4),羟胺(NH2OH),和亚硝酸盐(NO2-)],并估计它们的温度变化潜力,对三种中国农业土壤进行了异位干化试验。我们发现HONO和NOx(NO+NO2)的排放主要取决于NO2-,NH4+和NH2OH刺激NH3和N2O排放,分别。添加3,4-二甲基吡唑磷酸盐(DMPP)和乙炔显着降低了HONO和NOx的排放,在碱性Fluvo-Aquic土壤中,NH3排放显着增加。这些结果表明,氨氧化细菌(AOB)和完全氨氧化细菌(ComammoxNitrospira)在碱性Fluvo-aquic土壤中占主导地位的HONO和NOx排放,而氨氧化古细菌(AOA)在酸性Mollisol中占主导地位。DMPP有效减轻了Fluvo-水生土壤和Ultisol的变暖效应。总之,我们的发现强调了NO2-显著刺激了旱地农业土壤的HONO和NOx排放,以硝化为主。此外,土壤NH3、N2O、HONO,NOx排放表明不同的N周转过程,并应在生物地球化学和大气化学模型中加以考虑。
    The long-lived greenhouse gas nitrous oxide (N2O) and short-lived reactive nitrogen (Nr) gases such as ammonia (NH3), nitrous acid (HONO), and nitrogen oxides (NOx) are produced and emitted from fertilized soils and play a critical role for climate warming and air quality. However, only few studies have quantified the production and emission potentials for long- and short-lived gaseous nitrogen (N) species simultaneously in agricultural soils. To link the gaseous N species to intermediate N compounds [ammonium (NH4+), hydroxylamine (NH2OH), and nitrite (NO2-)] and estimate their temperature change potential, ex-situ dry-out experiments were conducted with three Chinese agricultural soils. We found that HONO and NOx (NO + NO2) emissions mainly depend on NO2-, while NH3 and N2O emissions are stimulated by NH4+ and NH2OH, respectively. Addition of 3,4-dimethylpyrazole phosphate (DMPP) and acetylene significantly reduced HONO and NOx emissions, while NH3 emissions were significantly enhanced in an alkaline Fluvo-aquic soil. These results suggested that ammonia-oxidizing bacteria (AOB) and complete ammonia-oxidizing bacteria (comammox Nitrospira) dominate HONO and NOx emissions in the alkaline Fluvo-aquic soil, while ammonia-oxidizing archaea (AOA) are dominant in the acidic Mollisol. DMPP effectively mitigated the warming effect in the Fluvo-aquic soil and the Ultisol. In conclusion, our findings highlight NO2- significantly stimulates HONO and NOx emissions from dryland agricultural soils, dominated by nitrification. In addition, subtle differences of soil NH3, N2O, HONO, and NOx emissions indicated different N turnover processes, and should be considered in biogeochemical and atmospheric chemistry models.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    尽管在政策驱动下减少了燃料燃烧中氮氧化物(NOx)的排放,但自2013年以来,中国夏季地表臭氧一直在增加。在这里,我们研究了土壤活性氮(Nr,包括2013-2019年华北平原(NCP)臭氧增加中的NOx和亚硝酸(HONO))排放量,使用GEOS-Chem化学输运模型模拟。我们根据观测约束的参数化方案更新了GEOS-Chem中的土壤NOx排放并添加了土壤HONO排放。该模型估计,2019年6月至7月,NCP的土壤Nr排放量为8.0ppbv,中国的5.5ppbv,导致每日最大8小时平均臭氧(MDA8)增强。我们确定了NCP地区燃烧和土壤Nr源对臭氧产生的强烈竞争作用。我们发现,土壤Nr排放使2013-2019年6月至7月的臭氧比NCP增加了3.0ppbv。土壤Nr臭氧贡献的增加,然而,主要不是由天气引起的土壤Nr排放增加驱动的,但是由于燃料燃烧NOx排放的同时减少,通过将臭氧生产推向对NOx更敏感的状态来提高土壤中的臭氧生产效率。我们的结果揭示了通过增加土壤Nr排放产生的臭氧,燃料燃烧NOx减排对臭氧趋势的重要间接影响,强调在华北平原臭氧缓解中考虑人为源和生物源之间相互作用的必要性。
    Summertime surface ozone in China has been increasing since 2013 despite the policy-driven reduction in fuel combustion emissions of nitrogen oxides (NOx). Here we examine the role of soil reactive nitrogen (Nr, including NOx and nitrous acid (HONO)) emissions in the 2013-2019 ozone increase over the North China Plain (NCP), using GEOS-Chem chemical transport model simulations. We update soil NOx emissions and add soil HONO emissions in GEOS-Chem based on observation-constrained parametrization schemes. The model estimates significant daily maximum 8 h average (MDA8) ozone enhancement from soil Nr emissions of 8.0 ppbv over the NCP and 5.5 ppbv over China in June-July 2019. We identify a strong competing effect between combustion and soil Nr sources on ozone production in the NCP region. We find that soil Nr emissions accelerate the 2013-2019 June-July ozone increase over the NCP by 3.0 ppbv. The increase in soil Nr ozone contribution, however, is not primarily driven by weather-induced increases in soil Nr emissions, but by the concurrent decreases in fuel combustion NOx emissions, which enhance ozone production efficiency from soil by pushing ozone production toward a more NOx-sensitive regime. Our results reveal an important indirect effect from fuel combustion NOx emission reduction on ozone trends by increasing ozone production from soil Nr emissions, highlighting the necessity to consider the interaction between anthropogenic and biogenic sources in ozone mitigation in the North China Plain.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

公众号