environmental chemistry

环境化学
  • 文章类型: Journal Article
    遵循在奥斯陆举行的第16届国际化学与环境会议(ICCE)的传统,挪威(2017年),以及随后在塞萨洛尼基举行的第17届ICCE,希腊(2019年),在威尼斯举行的第18届ICCE上组织了一次关于环境科学高等教育的后续会议,意大利(2023年6月)。会议的目的是促进就研究生和研究生教育方案交流经验和知识,包括他们的发展,优先次序,和执行。会议讨论了实践培训活动的整合,其中包括环境化学在各种学士和硕士课程的整合。目的是证明环境化学作为跨学科科学学科的多功能性,可以开发必要的绿色技能,为明天的环境专家制定可持续战略。此外,会议期间,与会者进行了一项调查,收集听众对环境化学教育(及相关领域)的态度和看法。
    Following the tradition of the 16th International Conference on Chemistry and the Environment (ICCE) in Oslo, Norway (2017), and the subsequent 17th ICCE in Thessaloniki, Greece (2019), a follow-up session on higher education in environmental science was organized at the 18th ICCE in Venice, Italy (June 2023). The aim of the session was to stimulate the exchange of experiences and knowledge on graduate and post-graduate level educational programmes, including their development, prioritization, and implementation. The session discussed the integration of practical training activities, which included the integration of environmental chemistry in various bachelor\'s and master\'s programmes. The aim was to demonstrate the versatility of environmental chemistry as an interdisciplinary scientific discipline that allows the development of essential green skills for developing sustainable strategies for the environmental experts of tomorrow. Furthermore, during the session, a survey was conducted among the conference participants to collect attitudes and reflections from the audience on the education of environmental chemistry (and related fields).
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  • 文章类型: Journal Article
    光电催化高级氧化过程(PEAOP)需要高性能和稳定的光阳极来有效氧化工业废水中的复杂污染物。本研究提出了2DWO3/MXene异壬基结构的构建,用于开发高效稳定的光阳极。WO3/MXene异质结构具有固定在微米大小的MXene片上的有序WO3光敏位点,为污染物氧化提供增加的可见光活性催化表面积和增强的电催化活性。苯酚,一种剧毒的化合物,在0.8V的施加电位下完全氧化可见光照射下的RHE。对苯酚光电催化氧化的操作条件进行了系统优化。通过高效液相色谱(HPLC)分析和中间体化合物的鉴定阐明了苯酚的氧化机理。此外,污染水中苯酚和砷(III)的混合模型证明了WO3/MXene光电阳极同时氧化有机和无机污染物的能力,实现苯酚和As(III)向无毒As(V)的完全转化。WO3/MXene光阳极促进水氧化,产生大量的O2·-和·OH氧化物质,这对于苯酚和砷的同时氧化至关重要。可回收性测试表明,性能保持了99%,确认WO3/MXene光电阳极在PEAOPs中长期运行的适用性。研究结果表明,将WO3/MXene光阳极集成到水净化系统中可以提高经济可行性,降低能耗,提高效率。该PEAOP为各种水体中重金属和有机化学污染的关键问题提供了可行的解决方案,鉴于其可扩展性和在保护清洁水资源的同时保护生态系统的能力。
    The photoelectrocatalytic advanced oxidation process (PEAOP) necessitates high-performing and stable photoanodes for the effective oxidation of complex pollutants in industrial wastewater. This study presents the construction of 2D WO3/MXene heteronanostructures for the development of efficient and stable photoanode. The WO3/MXene heterostructure features well-ordered WO3 photoactive sites anchored on micron-sized MXene sheets, providing an increased visible light active catalytic surface area and enhanced electrocatalytic activities for pollutant oxidation. Phenol, a highly toxic compound, was completely oxidized at an applied potential of 0.8 V vs. RHE under visible light irradiation. Systematic optimization of operational conditions for the photoelectrocatalytic oxidation of phenol was conducted. The phenol oxidation mechanism was elucidated via high-performance liquid chromatography (HPLC) analysis and the identification of intermediate compounds. Additionally, a mixed model of phenol and arsenic (III) in polluted water demonstrated the capability of WO3/MXene photoanode for the simultaneous oxidation of both organic and inorganic pollutants, achieving complete conversion of phenol and As(III) to non-toxic As(V). The WO3/MXene photoanode facilitated water oxidation, generating a substantial amount of O2•- and •OH oxidative species, which are crucial for the concurrent oxidation of phenol and arsenic. Recyclability tests demonstrated a 99% retention of performance, confirming the WO3/MXene photoanode\'s suitability for long-term operation in PEAOPs. The findings suggest that integrating WO3/MXene photoanodes into water purification systems can enhance economic feasibility, reduce energy consumption, and improve efficiency. This PEAOP offers a viable solution to the critical issue of heavy metal and organic chemical pollution in various water bodies, given its scalability and ability to preserve ecosystems while conserving clean water resources.
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  • 文章类型: Journal Article
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  • 文章类型: Journal Article
    X射线无定形材料包含15-73重量%。盖尔陨石坑中沉积岩和风成沉积物的百分比。这种材料是不同的硅质和富铁,但贫铝。挥发物的存在与初期风化产物的存在是一致的。为了更好地理解这种物质对火星上过去的含水条件的影响,在这里,我们使用批量和选择性溶解方法研究了不同年龄和环境条件的陆地富铁土壤中X射线无定形物质的形成和寿命,X射线衍射,和透射电子显微镜。结果表明,需要原位水蚀以将铁浓缩成粘土级分料。较冷的气候促进X射线无定形材料的形成和持久性,而较热的气候促进结晶次生相的形成。因此,火星上富含铁的X射线非晶态物质的形成和持久性与过去的凉爽和相对潮湿的环境以及长期的寒冷和干燥条件一致。
    X-ray amorphous material comprises 15-73 wt.% of sedimentary rocks and eolian sediments in Gale crater. This material is variably siliceous and iron rich but aluminum poor. The presence of volatiles is consistent with the existence of incipient weathering products. To better understand the implications of this material for past aqueous conditions on Mars, here we investigate X-ray amorphous material formation and longevity within terrestrial iron rich soils with varying ages and environmental conditions using bulk and selective dissolution methods, X-ray diffraction, and transmission electron microscopy. Results indicate that in situ aqueous alteration is required to concentrate iron into clay-size fraction material. Cooler climates promote the formation and persistence of X-ray amorphous material whereas warmer climates promote the formation of crystalline secondary phases. Iron rich X-ray amorphous material formation and persistence on Mars are therefore consistent with past cool and relatively wet environments followed by long-term cold and dry conditions.
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  • 文章类型: Journal Article
    可见光驱动的过氧化氢(H2O2)的光催化生产是目前将太阳能转化为化学能的新兴方法。总的来说,光催化生产H2O2的过程包括两个途径:水氧化反应(WOR)和氧还原反应(ORR)。然而,ORR的利用效率超过WOR,导致与天然水中低氧水平的差异,从而阻碍了它们的实际应用。在这里,我们报道了一种新型的供体-桥-受体(D-B-A)有机聚合物,通过Sonogashira-Hagihara偶联反应与四苯基乙烯(TPE)单元作为电子供体,乙炔(A)作为连接体,芘(P)部分作为电子受体。值得注意的是,所得的TPE-A-P表现出1.65%的显着太阳能到化学转化率和高BET比表面积(1132m2·g-1)。此外,即使在厌氧条件下,它显示出令人印象深刻的H2O2光合效率为1770μmolg-1h-1,超过了先前报道的绝大多数H2O2光合系统。出色的性能归因于电子和空穴的有效分离,随着足够的反应位点的存在促进了炔基电子桥的结合。该协议提出了一种通过水氧化反应产生H2O2的成功方法,标志着在自然环境中的实际应用取得了重大进展。
    The visible-light-driven photocatalytic production of hydrogen peroxide (H2O2) is currently an emerging approach for transforming solar energy into chemical energy. In general, the photocatalytic process for producing H2O2 includes two pathways: the water oxidation reaction (WOR) and the oxygen reduction reaction (ORR). However, the utilization efficiency of ORR surpasses that of WOR, leading to a discrepancy with the low oxygen levels in natural water and thereby impeding their practical application. Herein, we report a novel donor-bridge-acceptor (D-B-A) organic polymer conjugated by the Sonogashira-Hagihara coupling reaction with tetraphenylethene (TPE) units as the electron donors, acetylene (A) as the connectors and pyrene (P) moieties as the electron acceptors. Notably, the resulting TPE-A-P exhibits a remarkable solar-to-chemical conversion of 1.65% and a high BET-specific surface area (1132 m2·g-1). Furthermore, even under anaerobic conditions, it demonstrates an impressive H2O2 photosynthetic efficiency of 1770 μmol g-1 h-1, exceeding the vast majority of previously reported photosynthetic systems of H2O2. The outstanding performance is attributed to the effective separation of electrons and holes, along with the presence of sufficient reaction sites facilitated by the incorporation of alkynyl electronic bridges. This protocol presents a successful method for generating H2O2 via a water oxidation reaction, signifying a significant advancement towards practical applications in the natural environment.
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  • 文章类型: Journal Article
    被动采样器是采样水中亲水性微污染物的关键工具。两种主要方法解决了流体动力学的影响:(1)通过表征kw来确定特定地点的采样率(RS),水边界层(WBL)的传质系数,和(2)使用扩散材料减少WBL冲击以控制吸收。第一个需要校准数据,第二个仅使用易碎的扩散材料实现。这项研究评估了亲水性污染物通过聚四氟乙烯(PTFE;30µm厚)的转移,一种新的膜材料,具有比常用的聚醚砜(PES)更低的吸附。首次以类似Chemcatcher的配置组合,我们校准了44个微污染物的改良采样器,以提供RS-kw关系,用于原位RS测定(方法1)。微污染物在吸附剂上的积累比在PTFE上的积累多2000倍。基于PTFE的RS(0.027至0.300Lday-1)比先前报道的PES高2.5。膜性能测量(孔隙率,弯曲)表明积累主要受膜控制。外推法表明,使用较厚的PTFE膜(≥100µm)会在河流条件下将吸收控制完全转移到膜上(方法2)。这一发现可以实现基于污染物特性的RS预测,因此代表了被动采样的显著进步。
    Passive samplers are key tools to sample hydrophilic micropollutants in water. Two main approaches address the influence of hydrodynamics: (1) determining site-specific sampling rate (RS) by characterizing kw, the mass transfer coefficient of the water-boundary layer (WBL), and (2) reducing WBL impact using a diffusive material to control the uptake. The first requires calibration data and the second has only been achieved using fragile diffusive material. This study assesses the transfer of hydrophilic contaminants through polytetrafluoroethylene (PTFE; 30 µm thick), a new membrane material with lower sorption than commonly used polyethersulfone (PES). Combined for the first time in a Chemcatcher-like configuration, we calibrated the modified samplers for 44 micropollutants to provide RS - kw relationships for in-situ RS determination (approach 1). Micropollutants accumulated over 2000 times more on the sorbent than on PTFE. PTFE-based RS (0.027 to 0.300 L day-1) were 2.5 higher than previously reported with PES. Membrane property measurements (porosity, tortuosity) indicated that accumulation is primarily controlled by the membrane. Extrapolation indicated that using thicker PTFE membranes (≥ 100 µm) would shift uptake control entirely to the membrane in river conditions (approach 2). This finding could enable RS prediction based on contaminants properties, thus representing a significant advancement in passive sampling.
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  • 文章类型: Journal Article
    社会和科学的进步导致了新的学习计划的形成,通常是多学科课程。此类课程的担保人和教师必须做好准备,以迅速适应学生的需求和要求,社会,就业市场,和商业领域,因为许多问题在项目生命的最初几年开始浮出水面。在这里,我们分享了自2019年以来在布尔诺的Masaryk大学教授的“环境与健康”学习计划中这样一个过程的经验,捷克共和国。学生和校友的反馈可以改善课程和组织。我们从三个角度展示了反馈循环:来自即时短期经验的反馈可以在一年内纳入,中期反馈循环可以在几年后显现,和长期的甚至几十年。虽然目前的学生通常只感知短期或中期问题,该计划的哲学和结构必须通过预测未来几十年的社会和商业需求来建立。这样的长期方面往往与学生的愿景背道而驰,但仍然必须考虑该计划对新申请人保持吸引力。平衡最初的愿景,准备和应用更改,处理各级反馈是成功学习计划的关键管理挑战。
    Societal and scientific progress has led to the formation of new study programs, often with multidisciplinary curricula. Guarantors and teachers of such programs must be prepared to quickly adapt to the needs and demands of students, society, the job market, and the commercial sphere since many issues start surfacing during the first years of the programs\' life. Here we share our experience with such a process in the study program \"Environment and Health\" taught since 2019 at Masaryk University in Brno, Czech Republic. Feedback from students and alumni allows for improvement of the curriculum and organization of the program. We show feedback loops from three perspectives: Feedback from immediate short-term experience can be incorporated within a year, medium-term feedback loops can manifest after several years, and long-term ones even decades. While current students usually perceive only short- or medium-term issues, the philosophy and structure of the program must be built by predicting societal and commercial needs in the following decades. Such long-term aspects are often counterintuitive to students\' vision, but still have to be considered for the program to remain attractive to new applicants. Balancing the original vision, preparing and applying changes, and dealing with feedback on all levels are key managerial challenges of successful study programs.
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  • 文章类型: Journal Article
    将废锂离子电池(LIBs)正极材料转化为环境催化剂已引起越来越多的关注。在这里,我们用废LiCoO2LIBs(Co3O4-LIBs)制造了Co3O4基催化剂,发现集电器中Al和Cu对其性能的作用是不可忽略的。密度泛函理论计算证实,Al和/或Cu的掺杂使Co的d带中心上移。采用基于过氧单硫酸盐(PMS)活化的类Fenton反应来评估其活性。有趣的是,铝掺杂增强了PMS的化学吸附(从-2.615eV到-2.623eV),并缩短了它们之间的Co-O键长(从2.540µ到2.344µ),而Cu掺杂降低了界面电荷转移电阻(从28.347kΩ降低到6.689kΩ),除了上述特性的增强。不出所料,Co3O4-LIB对双酚A的降解活性(0.523min-1)优于由商业CoC2O4制备的Co3O4(0.287min-1)。同时,通过比较将Al和/或Cu掺杂到Co3O4中的催化剂的活性,进一步证实了活性改善的原因。这项工作揭示了电流收集器中的元素对废旧LIB功能材料性能的作用,有利于废LIB的可持续利用。
    Converting spent lithium-ion batteries (LIBs) cathode materials into environmental catalysts has drawn more and more attention. Herein, we fabricated a Co3O4-based catalyst from spent LiCoO2 LIBs (Co3O4-LIBs) and found that the role of Al and Cu from current collectors on its performance is nonnegligible. The density functional theory calculations confirmed that the doping of Al and/or Cu upshifts the d-band center of Co. A Fenton-like reaction based on peroxymonosulfate (PMS) activation was adopted to evaluate its activity. Interestingly, Al doping strengthened chemisorption for PMS (from -2.615 eV to -2.623 eV) and shortened Co-O bond length (from 2.540 Å to 2.344 Å) between them, whereas Cu doping reduced interfacial charge-transfer resistance (from 28.347 kΩ to 6.689 kΩ) excepting for the enhancement of the above characteristics. As expected, the degradation activity toward bisphenol A of Co3O4-LIBs (0.523 min-1) was superior to that of Co3O4 prepared from commercial CoC2O4 (0.287 min-1). Simultaneously, the reasons for improved activity were further verified by comparing activity with catalysts doped Al and/or Cu into Co3O4. This work reveals the role of elements from current collectors on the performance of functional materials from spent LIBs, which is beneficial to the sustainable utilization of spent LIBs.
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  • 文章类型: Journal Article
    我们审查的主要目标是系统地探索和比较农药检测中采用的最先进的方法,全球食品安全倡议的重要组成部分。发光纳米传感器领域的新方法,色谱,太赫兹光谱,和拉曼光谱进行了精确的讨论,快速,以及食品和农业生态样品中农药检测的通用策略。发光纳米传感器成为强大的工具,以其便携性和无与伦比的灵敏度和实时监控能力而著称。液相和气相色谱法与光谱检测器耦合,分析化学领域的中坚力量,因其精确而受到称赞,广泛的适用性,并在不同的监管环境中进行验证。太赫兹光谱提供了独特的优势,如非侵入性测试,深刻的渗透深度,和批量样品处理。同时,拉曼光谱以其无损性质脱颖而出,它甚至能够检测到痕量的农药,和样品制备的最低要求。在承认这些技术的成熟度和鲁棒性的同时,我们的审查强调了持续创新的重要性。这些方法的意义超出了它们目前的功能,强调他们应对不断变化的挑战的适应性。环境毒物化学2024;00:1-17。©2024作者WileyPeriodicalsLLC代表SETAC出版的环境毒理学和化学。
    The primary goal of our review was to systematically explore and compare the state-of-the-art methodologies employed in the detection of pesticides, a critical component of global food safety initiatives. New approach methods in the fields of luminescent nanosensors, chromatography, terahertz spectroscopy, and Raman spectroscopy are discussed as precise, rapid, and versatile strategies for pesticide detection in food items and agroecological samples. Luminescent nanosensors emerge as powerful tools, noted for their portability and unparalleled sensitivity and real-time monitoring capabilities. Liquid and gas chromatography coupled to spectroscopic detectors, stalwarts in the analytical chemistry field, are lauded for their precision, wide applicability, and validation in diverse regulatory environments. Terahertz spectroscopy offers unique advantages such as noninvasive testing, profound penetration depth, and bulk sample handling. Meanwhile, Raman spectroscopy stands out with its nondestructive nature, its ability to detect even trace amounts of pesticides, and its minimal requirement for sample preparation. While acknowledging the maturity and robustness of these techniques, our review underscores the importance of persistent innovation. These methodologies\' significance extends beyond their present functions, highlighting their adaptability to meet ever-evolving challenges. Environ Toxicol Chem 2024;43:1468-1484. © 2024 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
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  • 文章类型: Journal Article
    全球氢氟碳化合物(HFC)制冷剂相下降的实施导致氢氟烯烃(HFO)作为低全球变暖潜能值(GWP)替代品的引入,考虑到他们的低大气寿命。然而,迄今为止,尚不完全清楚HFOs主要降解产物三氟乙醛(TFE)的长期大气命运,三氟乙酰氟(TFF),和三氟乙酸(TFA)。它特别涉及形成HFC-23的可能性,HFC-23是一种有效的全球变暖剂。虽然TFE的大气反应网络,TFF,TFA有相当的复杂性,相关的大气化学途径在文献中有很好的特点,能够对HFC-23的形成进行全面的危害评估,作为不同情况下的次要HFO分解产品。在基线情况下,HFO有效GWP的下限高于监管阈值。虽然进一步的研究对于完善气候风险评估至关重要,现有证据表明,与HFOs相关的气候危害不可忽视。
    The enforcement of a global hydrofluorocarbon (HFC) refrigerant phase down led to the introduction of hydrofluoroolefins (HFOs) as a low Global Warming Potential (GWP) substitute, given their low atmospheric lifetime. However, to this date it is not fully clear the long-term atmospheric fate of HFOs primary degradation products: trifluoro acetaldehyde (TFE), trifluoro acetyl fluoride (TFF), and trifluoroacetic acid (TFA). It particularly concerns the possibility of forming HFC-23, a potent global warming agent. Although the atmospheric reaction networks of TFE, TFF, and TFA have a fair level of complexity, the relevant atmospheric chemical pathways are well characterized in the literature, enabling a comprehensive hazard assessment of HFC-23 formation as a secondary HFO breakdown product in diverse scenarios. A lower bound of the HFOs effective GWP in a baseline scenario is found above regulatory thresholds. While further research is crucial to refine climate risk assessments, the existing evidence suggests a non-negligible climate hazard associated with HFOs.
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