Polycyclic aromatic hydrocarbons

多环芳烃
  • 文章类型: Journal Article
    UNASSIGNED: Exposure to environmental chemicals such as phthalates, phenols, and polycyclic aromatic hydrocarbons (PAHs) during pregnancy can increase the risk of adverse newborn outcomes. We explored the associations between maternal exposure to select environmental chemicals and DNA methylation in cord blood mononuclear cells (CBMC) and placental tissue (maternal and fetal sides) to identify potential mechanisms underlying these associations.
    UNASSIGNED: This study included 75 pregnant individuals who planned to give birth at the University of Cincinnati Hospital between 2014 and 2017. Maternal urine samples during the delivery visit were collected and analyzed for 37 biomarkers of phenols (12), phthalates (13), phthalate replacements (4), and PAHs (8). Cord blood and placenta tissue (maternal and fetal sides) were also collected to measure the DNA methylation intensities using the Infinium HumanMethylation450K BeadChip. We used linear regression, adjusting for potential confounders, to assess CpG-specific methylation changes in CBMC (n = 54) and placenta [fetal (n = 67) and maternal (n = 68) sides] associated with gestational chemical exposures (29 of 37 biomarkers measured in this study). To account for multiple testing, we used a false discovery rate q-values < 0.05 and presented results by limiting results with a genomic inflation factor of 1±0.5. Additionally, gene set enrichment analysis was conducted using the Kyoto Encyclopedia of Genes and Genomics pathways.
    UNASSIGNED: Among the 29 chemical biomarkers assessed for differential methylation, maternal concentrations of PAH metabolites (1-hydroxynaphthalene, 2-hydroxyfluorene, 4-hydroxyphenanthrene, 1-hydroxypyrene), monocarboxyisononyl phthalate, mono-3-carboxypropyl phthalate, and bisphenol A were associated with altered methylation in placenta (maternal or fetal side). Among exposure biomarkers associated with epigenetic changes, 1-hydroxynaphthalene, and mono-3-carboxypropyl phthalate were consistently associated with differential CpG methylation in the placenta. Gene enrichment analysis indicated that maternal 1-hydroxynaphthalene was associated with lipid metabolism and cellular processes of the placenta. Additionally, mono-3-carboxypropyl phthalate was associated with organismal systems and genetic information processing of the placenta.
    UNASSIGNED: Among the 29 chemical biomarkers assessed during delivery, 1-hydroxynaphthalene and mono-3-carboxypropyl phthalate were associated with DNA methylation in the placenta.
    UNASSIGNED: The online version contains supplementary material available at 10.1186/s43682-024-00027-7.
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  • 文章类型: Journal Article
    OBJECTIVE: Prenatal exposure to polycyclic aromatic hydrocarbons (PAHs) is associated with adverse birth and developmental outcomes in children. We aimed to describe prenatal PAH exposures in a large, multisite U.S. consortium.
    METHODS: We measured 12 mono-hydroxylated metabolites (OH-PAHs) of 7 PAHs (naphthalene, fluorene, phenanthrene, pyrene, benzo(c)phenanthrene, chrysene, benz(a)anthracene) in mid-pregnancy urine of 1,892 pregnant individuals from the ECHO PATHWAYS consortium cohorts: CANDLE (n = 988; Memphis), TIDES (n = 664; Minneapolis, Rochester, San Francisco, Seattle) and GAPPS (n = 240; Seattle and Yakima, WA). We described concentrations of 8 OH-PAHs of non-smoking participants (n = 1,695) by site, socioeconomic characteristics, and pregnancy stage (we report intraclass correlation coefficients (ICC) for n = 677 TIDES participants).
    RESULTS: Exposure to the selected PAHs was ubiquitous at all sites. 2-hydroxynaphthalene had the highest average concentrations at all sites. CANDLE had the highest average concentrations of most metabolites. Among non-smoking participants, we observed some patterns by income, education, and race but these were not consistent and varied by site and metabolite. ICCs of repeated OH-PAH measures from TIDES participants were ≤ 0.51.
    CONCLUSIONS: In this geographically-diverse descriptive analysis of U.S. pregnancies, we observed ubiquitous exposure to low molecular weight PAHs, highlighting the importance of better understanding PAH sources and their pediatric health outcomes attributed to early life PAH exposure.
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  • 文章类型: Journal Article
    在实弹训练期间,消防教官不可避免地暴露于萘等多环芳烃(PAHs)。该研究旨在通过测量萘代谢物1,2-二羟基萘(DHN)的尿排泄来研究萘的摄取,描述DHN消除动力学,并通过与进一步的PAH暴露生物标志物进行比较来评估结果。N=6名男性禁烟消防教官在呼吸保护下的住宅火灾模拟单元中分别完成了五次培训课程。所有参与者在每次会议之前提供了两个尿液样本,在每次会议后的18小时间隔内提供了另外七个样本。通过气相色谱/串联质谱法(GC-MS/MS)在所有样品(n=237)中检测到DHN,中位浓度范围为3.3µg/gcrea。(范围0.9-10.2)在暴露于134.2µg/gcrea之前。(43.4-380.4)暴露后。暴露开始后3.3h发现的最大消除(中位数)减少,平均半衰期为6.6h至27.1µg/gcrea。(15.7-139.5)训练后18小时。DHN敏感地表明在训练期间假定真皮萘摄入量,表现出与其他萘代谢物相似的消除动力学。参与者的内部暴露暂时超过了普通人群中确定的非吸烟者的暴露量,但低于其他有PAH暴露的工作场所。尽管吸收有限,积累是可能的日常接触。
    Exposure of firefighting instructors to polycyclic aromatic hydrocarbons (PAHs) such as naphthalene is unavoidable during live fire training. The study aimed to investigate naphthalene uptake by measuring the urinary excretion of the naphthalene metabolite 1,2-dihydroxynaphthalene (DHN), to describe the DHN elimination kinetics and to evaluate the results by comparison to further biomarkers of PAH exposure. N = 6 male non-smoking firefighting instructors completed five training sessions each in a residential fire simulation unit under respiratory protection. All participants provided two urine samples before and another seven samples within an 18-h-interval after each session. DHN was detected by gas chromatography/tandem mass spectrometry (GC-MS/MS) in all samples (n = 237) with median concentrations ranging from 3.3 µg/g crea. (range 0.9-10.2) before exposure to 134.2 µg/g crea. (43.4-380.4) post exposure. Maximum elimination found 3.3 h (median) after onset of exposure decreased with a mean half-life of 6.6 h to 27.1 µg/g crea. (15.7-139.5) 18 h after training. DHN sensitively indicated a presumed dermal naphthalene intake during training, showing similar elimination kinetics like other naphthalene metabolites. Internal exposure of the participants transiently exceeded exposures determined for non-smokers in the general population, but was lower than at other workplaces with PAH exposure. Despite limited uptake, accumulation is possible with daily exposure.
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  • 文章类型: Journal Article
    本研究旨在开发一种由磁性壳聚糖/二硫化钼(CS/MoS2/Fe3O4)组成的高效纳米复合材料,用于去除三种多环芳烃(PAHs)-芘,蒽,还有菲.通过创新的合成程序和利用磁性来增强吸附能力,引入了新颖性。此外,强调了壳聚糖作为吸附剂成分的绿色性,与传统吸附剂相比,突出了其可生物降解性和低环境影响。影响PAH吸附的因素,如纳米复合材料用量,PAH初始浓度,pH值,和接触时间,进行了系统的研究和优化。结果表明,当PAH的初始浓度为150mg/L时,可以达到最佳的去除效果。吸附剂剂量为0.045g,pH为6.0,接触时间为150分钟。伪二级动力学模型表现出优于实验数据的拟合,表示约150分钟的平衡时间。此外,平衡吸附过程遵循Freundlich等温线模型,kf和n值分别超过7.91mg/g和1.20。值得注意的是,菲的最大吸收能力,蒽,吸附剂上的芘测定为217mg/g,204mg/g,222毫克/克,分别。这些发现强调了CS/MoS2/Fe3O4纳米复合材料在有效去除牛奶和其他乳制品中的PAHs的巨大潜力,从而有助于改善食品安全和公共卫生。
    This study aimed to develop a highly efficient nanocomposite composed of magnetic chitosan/molybdenum disulfide (CS/MoS2/Fe3O4) for the removal of three polycyclic aromatic hydrocarbons (PAHs)-pyrene, anthracene, and phenanthrene. Novelty was introduced through the innovative synthesis procedure and the utilization of magnetic properties for enhanced adsorption capabilities. Additionally, the greenness of chitosan as a sorbent component was emphasized, highlighting its biodegradability and low environmental impact compared to traditional sorbents. Factors influencing PAH adsorption, such as nanocomposite dosage, initial PAH concentration, pH, and contact time, were systematically investigated and optimized. The results revealed that optimal removal efficiencies were attained at an initial PAH concentration of 150 mg/L, a sorbent dose of 0.045 g, pH 6.0, and a contact time of 150 min. The pseudo-second-order kinetic model exhibited superior fitting to the experimental data, indicating an equilibrium time of approximately 150 min. Moreover, the equilibrium adsorption process followed the Freundlich isotherm model, with kf and n values exceeding 7.91 mg/g and 1.20, respectively. Remarkably, the maximum absorption capacities for phenanthrene, anthracene, and pyrene on the sorbent were determined as 217 mg/g, 204 mg/g, and 222 mg/g, respectively. These findings underscore the significant potential of the CS/MoS2/Fe3O4 nanocomposite for efficiently removing PAHs from milk and other dairy products, thereby contributing to improved food safety and public health.
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  • 文章类型: Journal Article
    探索具有优异电化学发光性能的新型ECL发光体是当前ECL领域的研究热点。在这里,通过以多孔超薄Zr-BTB金属有机层(MOL)为载体,配位接枝廉价易得的多环芳烃(PAH)衍生物发光基团PyTS,制备了一种新型的高效无Ru络合物的ECL发射体PyTS-Zr-BTB-MOL,其ECL性能从未被研究过。令人欣喜的是,与PyTS单体和PyTS聚集体相比,PyTS-Zr-BTB-MOL的ECL强度和效率显着增强。主要原因是PyTS接枝在Zr-BTB-MOL的Zr6团簇上后,芘环之间的距离大大扩大,克服了PyTS的聚集引起的猝灭(ACQ)效应,从而增强了ECL发射。同时,PyTS-Zr-BTB-MOL的多孔纳米片结构可以明显增加PyTS发光体的暴露量,缩短共反应物和电子/离子的扩散路径,这有效地促进了更多PyTS发光体的电化学激发,从而实现了进一步的ECL增强。鉴于PyTS-Zr-BTB-MOL的显著ECL特性,它被用作ECL指示剂,以构建用于microRNA-21测定的新型高灵敏度ECL生物传感器,具有令人满意的响应范围(100aM至100pM)和超低检测限(10.4aM)。总的来说,这项工作表明,使用MOL协同接枝PAH衍生发光体以消除ACQ效应并提高发光体的利用率是开发用于组装超灵敏ECL生物传感平台的高性能无Ru络合物ECL材料的一种有前途且有效的策略。
    The exploration of novel electrochemiluminescence (ECL) luminophores with excellent ECL properties is a current research hotspot in the ECL field. Herein, a novel high-efficiency Ru-complex-free ECL emitter PyTS-Zr-BTB-MOL has been prepared by using porous ultrathin Zr-BTB metal-organic layer (MOL) as carrier to coordinatively graft the cheap and easily available polycyclic aromatic hydrocarbon (PAH) derivative luminophore PyTS whose ECL performance has never been investigated. Gratifyingly, the ECL intensity and efficiency of PyTS-Zr-BTB-MOL were markedly enhanced compared to both PyTS monomers and PyTS aggregates. The main reason was that the distance between pyrene rings was greatly expanded after the PyTS grafting on the Zr6 clusters of Zr-BTB-MOL, which overcame the aggregation-caused quenching (ACQ) effect of PyTS and thus enhanced the ECL emission. Meanwhile, the porous nanosheet structure of PyTS-Zr-BTB-MOL could distinctly increase the exposure of PyTS luminophores and shorten the diffusion paths of coreactants and electrons/ions, which effectively promoted the electrochemical excitation of more PyTS luminophores and thus achieved a further ECL enhancement. In light of the remarkable ECL property of PyTS-Zr-BTB-MOL, it was employed as an ECL indicator to build a novel high-sensitivity ECL biosensor for microRNA-21 determination, possessing a satisfactory response range (100 aM to 100 pM) and an ultralow detection limit (10.4 aM). Overall, this work demonstrated that using MOLs to coordinatively graft the PAH derivative luminophores to eliminate the ACQ effect and increase the utilization rate of the luminophores is a promising and efficient strategy to develop high-performance Ru-complex-free ECL materials for assembling ultrasensitive ECL biosensing platforms.
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  • 文章类型: Journal Article
    化学氧化结合微生物修复技术对多环芳烃(PAHs)的去除受到广泛关注。其中,精确评价PAH污染土壤的可行氧化剂浓度是实现土壤功能生态修复目标的关键。在这项研究中,菲(PHE)被用作目标污染物,Fe2激活的过硫酸盐(PS)用于修复四种类型的土壤。线性回归分析确定了影响修复的以下重要因素:PS用量和土壤PHE含量对PHE降解的影响,Fe2+用量,可水解氮(HN),和有效磷用于PS分解。建立了具有较高预测精度的“土壤特征-氧化条件-修复效果”综合模型。基于模型识别,绿脓杆菌GZ7驯化后具有较高的PAHs降解能力,进一步应用于耦合修复修复。结果表明,最佳PS剂量为0.75%(w/w)。土壤物理之间的响应关系,化学,分析了中间界面和氧化条件下的生物指标。使用微生物多样性测序阐明了耦合修复效果。铜绿假单胞菌GZ7的引入刺激了Cohnella的相对丰度,肠杆菌,拟芽孢杆菌,和芽孢杆菌,可以促进修复过程中的物质代谢和能量转化。
    Chemical oxidation coupled with microbial remediation has attracted widespread attention for the removal of polycyclic aromatic hydrocarbons (PAHs). Among them, the precise evaluation of the feasible oxidant concentration of PAH-contaminated soil is the key to achieving the goal of soil functional ecological remediation. In this study, phenanthrene (PHE) was used as the target pollutant, and Fe2+-activated persulphate (PS) was used to remediate four types of soils. Linear regression analysis identified the following important factors influencing remediation: PS dosage and soil PHE content for PHE degradation, Fe2+ dosage, hydrolysable nitrogen (HN), and available phosphorus for PS decomposition. A comprehensive model of \"soil characteristics-oxidation conditions-remediation effect\" with a high predictive accuracy was constructed. Based on model identification, Pseudomonas aeruginosa GZ7, which had high PAHs degrading ability after domestication, was further applied to coupling repair remediation. The results showed that the optimal PS dose was 0.75% (w/w). The response relationship between soil physical, chemical, and biological indicators at the intermediate interface and oxidation conditions was analysed. Coupled remediation effects were clarified using microbial diversity sequencing. The introduction of Pseudomonas aeruginosa GZ7 stimulated the relative abundance of Cohnella, Enterobacter, Paenibacillus, and Bacillus, which can promote material metabolism and energy transformation during remediation.
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  • 文章类型: Journal Article
    法兰克福香肠用山毛榉熏制,橡木,和Alder,分别,用于阐明烟气化学成分对杂环胺(HA)和多环芳烃(PAHs)水平的潜在影响。结果表明,不同的木材类型显着影响食品基质中目标物质的分布。山毛榉烟熏样品的总游离HAs含量较低(5.98-6.80ng/g干重DW),PAH4(3.31-3.83ng/gDW),和PAH8(10.0-10.8ng/gDW),whereas的热解通常导致更高的危险残留物(8.26-9.19ng/gDW的总游离HAs,4.24-6.60ng/gDW的PAH4和14.1-23.3ng/gDW的PAH8)。此外,烟雾化学成分的差异归因于15种关键确定物质的比例不同。其中,两种醛(5-甲基糠醛和糠醛)和两种酚(苯酚和5-羟基麦芽酚)可能对熏制肉制品中的HA和PAHs的形成具有协同或竞争性抑制作用。
    The Frankfurter sausages smoked with beech, oak, and alder, respectively, were used to clarify the underlying impact of the smoke chemical composition on the levels of heterocyclic amines (HAs) and polycyclic aromatic hydrocarbons (PAHs). The result indicated that different wood types significantly affected the profiles of target substances in food matrices. The beech-smoked samples had lower contents of total free HAs (5.98-6.80 ng/g dry-weight-DW), PAH4 (3.31-3.83 ng/g DW), and PAH8 (10.0-10.8 ng/g DW), whereas the alder pyrolysis usually led to higher hazardous residues (8.26-9.19 ng/g DW of total free HAs, 4.24-6.60 ng/g DW of PAH4 and 14.1-23.3 ng/g DW of PAH8). In addition, the differences in smoke chemical composition were attributed to the different proportions of 15 key identified substances. Among them, two aldehydes (5-methyl-furfural & furfural) and two phenols (phenol & 5-hydroxymaltol) may have synergistic or competitive inhibitory effects on the formation of HAs and PAHs in smoked meat products.
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  • 文章类型: Journal Article
    多环芳烃是影响人类健康和环境的空气污染物,并且它们在室外和室内环境中的准确测定是重要的。这项研究提出了一种对环境空气中半挥发性化合物进行采样和分析的方法,重点是多环芳烃。用小容量泵(4.8m3)在未调节的固相萃取柱(IsoluteENV+)中收集。使用低容量泵在SPE墨盒中采样,可以在室内和室外环境中收集气体和颗粒相化合物。并且减少了所需的提取步骤的数量以及用于提取的溶剂体积。通过GC-MS/MS对提取后的16种US-EPA优先PAHs进行分析,PAHs的回收率为40-118%。在取样期间没有检测到穿透。此外,该方法包括储存测试,以评估可热封Kapac袋中SPE盒中PAHs的保存情况;模拟从采样地点到实验室的运输,和房间下的存储,不同时间间隔的寒冷和冰冻条件,取样后3个月。结果表明,浓度水平在不同的储存时间间隔和温度下保持恒定,萘和萘是唯一的例外,第一次显示高空白水平,后来在室温下显示高空白水平。方法定量极限,包括采样,储存和GC-MS/MS分析范围从萘的2000pgm-3和菲的300pgm-3到分子量较高和挥发性较低的PAHs的小于20.0pgm-3,如苯并[a]芘(LOQ=8.0pgm-3)。通过在城市背景空气条件下进行室内采样,检验了该方法的可行性,显示单个PAH浓度高于其方法定量极限4至10倍。
    Polycyclic aromatic hydrocarbons are air pollutants that affect the human health and the environment, and their accurate determination in outdoor and indoor environments is important. This study presents a methodology for sampling and analysis of semi-volatile compounds in ambient air with emphasis on the polycyclic aromatic hydrocarbons, collected with low-volume pumps (4.8 m3) in unconditioned solid phase extraction cartridges (Isolute ENV+). Sampling in SPE cartridges with low-volume pumps allows the collection of both gas and particulate phase compounds in indoor as well as outdoor environments, and reduces the number of extraction steps required as well as the solvent volume used for extraction. Analysis of the 16 US-EPA priority PAHs after extraction was conducted by GC-MS/MS with recoveries of the PAHs 40-118 %. No breakthrough was detected during sampling. Moreover, the methodology includes storage test to assess the conservation of PAHs in the SPE cartridges in heat-sealable Kapac bags; simulating transport from sampling sites to laboratory, and storage under room, cold and frozen conditions at different time-intervals, up to 3 months after sampling. The results showed that concentration levels remained constant across various storage time intervals and temperatures, with naphthalene and acenaphthylene being the only exceptions, showing high blank levels for the first and losses at room temperature for the later. The method quantification limits, including sampling, storage and GC-MS/MS analysis ranged from 2000 pg m-3 for naphthalene and 300 pg m-3 for phenanthrene to less than 20.0 pg m-3 for higher molecular and less volatile PAHs, such as benzo[a]pyrene (LOQ = 8.0 pg m-3). The feasibility of the method was tested by sampling indoors under urban background air conditions, showing individual PAH concentrations 4 to 10 times higher than their method quantification limits.
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  • 文章类型: Journal Article
    海洋碳氢化合物细菌可以使用多环芳烃作为碳和能源,这使得这些细菌对石油污染水域的生物修复非常有吸引力。然而,物种之间的基因组和代谢差异仍然是了解降解PAHs的进化和策略的研究主题。这项研究提出了红球菌MSA14,这是一种从下加利福尼亚州海洋沉积物中分离出的细菌,墨西哥,表现出对盐水环境的适应性,高水平的固有芘耐受性(>5gL-1),在27天内有效降解芘(0.2gL-1)30%。此外,通过使用萘和菲作为单独的碳源,该菌株具有多功能性。R.ruberMSA14的基因组测序揭示了一个跨越5.45Mbp的基因组,一个72kbp的质粒,和三个推定的巨质粒,长度在110和470Kbp之间。对R.ruberMSA14基因组的生物信息学分析揭示了56个基因,这些基因编码参与芳烃分解代谢的外周和中心途径的酶,烷烃,烯烃,和聚合物降解。在它的基因组中,R.ruberMSA14具有负责耐盐性和铁载体生产的基因。此外,R.ruberMSA14对13个参考基因组的基因组分析显示,所有比较的菌株都至少有一个基因参与烷烃和邻苯二酚降解途径。总的来说,生理测定和基因组分析表明,R.ruberMSA14是一种新的耐卤碱和碳氢化合物碎屑菌株,使其成为深入表征研究和生物修复过程的有希望的候选人,作为合成微生物联盟的一部分,以及更好地了解红球菌群的分解代谢潜力和功能多样性。
    Marine hydrocarbonoclastic bacteria can use polycyclic aromatic hydrocarbons as carbon and energy sources, that makes these bacteria highly attractive for bioremediation in oil-polluted waters. However, genomic and metabolic differences between species are still the subject of study to understand the evolution and strategies to degrade PAHs. This study presents Rhodococcus ruber MSA14, an isolated bacterium from marine sediments in Baja California, Mexico, which exhibits adaptability to saline environments, a high level of intrinsic pyrene tolerance (> 5 g L- 1), and efficient degradation of pyrene (0.2 g L- 1) by 30% in 27 days. Additionally, this strain demonstrates versatility by using naphthalene and phenanthrene as individual carbon sources. The genome sequencing of R. ruber MSA14 revealed a genome spanning 5.45 Mbp, a plasmid of 72 kbp, and three putative megaplasmids, lengths between 110 and 470 Kbp. The bioinformatics analysis of the R. ruber MSA14 genome revealed 56 genes that encode enzymes involved in the peripheral and central pathways of aromatic hydrocarbon catabolism, alkane, alkene, and polymer degradation. Within its genome, R. ruber MSA14 possesses genes responsible for salt tolerance and siderophore production. In addition, the genomic analysis of R. ruber MSA14 against 13 reference genomes revealed that all compared strains have at least one gene involved in the alkanes and catechol degradation pathway. Overall, physiological assays and genomic analysis suggest that R. ruber MSA14 is a new haloalkalitolerant and hydrocarbonoclastic strain toward a wide range of hydrocarbons, making it a promising candidate for in-depth characterization studies and bioremediation processes as part of a synthetic microbial consortium, as well as having a better understanding of the catabolic potential and functional diversity among the Rhodococci group.
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  • 文章类型: Journal Article
    我们描述了与各种拓扑的PAH系统相连的π扩展的膦环(4元P环)的合成。这些化合物被充分表征,包括X-射线衍射。聚芳族平台和P环对结构的影响,光学和氧化还原性质进行了实验和理论研究。尽管P中心和4元环都不参与HOMO或LUMO轨道,这两个结构特征在扭曲轨道对称性方面都有重要的调节作用,导致手性属性。立体异构P原子用作远程手性微扰器,以诱导聚芳族体系的圆偏振发光。不对称因素高度依赖于多芳族拓扑,如理论计算所支持。
    We describe the synthesis of π-extended phosphetene rings (4-member P-rings) flanked with PAH systems of various topologies. These compounds are fully characterized including X-ray diffraction. The impact of both the polyaromatic platform and the P-ring on the structure, and the optical and redox properties are investigated both experimentally and theoretically. Although neither the P centre nor the 4-membered ring significantly takes part in the HOMO or LUMO orbitals, both structural features have an important modulating role in distorting the symmetry of the orbitals, leading to chiroptical properties. The stereogenic P-atom is used as a remote chiral perturbator to induce circularly polarized luminescence of the polyaromatic system. The dissymmetry factor is highly dependent on the polyaromatic topology, as supported by theoretical calculations.
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