ACS Earth and Space Chemistry最新文献

筛选
英文 中文
Cosmic Ray Irradiation of Interstellar Ices on Sulfur-Rich Grains: A Possible Source of Sulfur-Bearing Molecules 宇宙射线照射富硫颗粒上的星际冰:含硫分子的可能来源
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-05-07 DOI: 10.1021/acsearthspacechem.5c0003610.1021/acsearthspacechem.5c00036
Duncan V. Mifsud*, Zuzana Kaňuchová, Olivier Auriacombe, Péter Herczku, Danna Qasim, Sándor T. S. Kovács, Richárd Rácz, Béla Sulik, Zoltán Juhász, István Rajta, István Vajda, Sándor Biri, Robert W. McCullough, Sergio Ioppolo, Ujjwal Raut and Nigel J. Mason*, 
{"title":"Cosmic Ray Irradiation of Interstellar Ices on Sulfur-Rich Grains: A Possible Source of Sulfur-Bearing Molecules","authors":"Duncan V. Mifsud*,&nbsp;Zuzana Kaňuchová,&nbsp;Olivier Auriacombe,&nbsp;Péter Herczku,&nbsp;Danna Qasim,&nbsp;Sándor T. S. Kovács,&nbsp;Richárd Rácz,&nbsp;Béla Sulik,&nbsp;Zoltán Juhász,&nbsp;István Rajta,&nbsp;István Vajda,&nbsp;Sándor Biri,&nbsp;Robert W. McCullough,&nbsp;Sergio Ioppolo,&nbsp;Ujjwal Raut and Nigel J. Mason*,&nbsp;","doi":"10.1021/acsearthspacechem.5c0003610.1021/acsearthspacechem.5c00036","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00036https://doi.org/10.1021/acsearthspacechem.5c00036","url":null,"abstract":"<p >The major reservoir of sulfur in dense interstellar clouds is still largely unknown, although a growing body of evidence suggests that it may exist in a refractory form (i.e., as minerals or allotropes of the element). Therefore, it is possible that the irradiation of sulfur-free interstellar ices on top of sulfur-rich refractory grain components by cosmic rays or stellar winds may result in the formation of simple inorganic sulfur molecules that could be readily detected by ground- or space-borne telescopes. In this study, we have irradiated neat ices of O<sub>2</sub>, CO, CO<sub>2</sub>, and H<sub>2</sub>O on top of layers of allotropic sulfur at 20 K using 1 MeV He<sup>+</sup> ions as a mimic of space radiation. Experiments with CO<sub>2</sub> and H<sub>2</sub>O ices were also repeated at 70 K to provide data obtained under conditions more relevant to icy bodies in the outer solar system for comparative purposes. We have found qualitative mid-infrared spectroscopic evidence for the synthesis of SO<sub>2</sub>, CS<sub>2</sub>, OCS, and H<sub>2</sub>SO<sub>4</sub> hydrates, but not H<sub>2</sub>S, in our experiments and have quantified the efficiency of their formation by calculating the <i>G</i>-value (i.e., the number of molecules formed per 100 eV of energy deposited) for each ice-refractory system. Overall, SO<sub>2</sub> and CS<sub>2</sub> are the most commonly observed products in our experiments, although the highest <i>G</i>-value was that for H<sub>2</sub>SO<sub>4</sub> hydrates formed as a result of the irradiation of H<sub>2</sub>O ice on top of sulfur at 70 K. An important outcome of our study is that our experimental results are consistent with recent observational surveys that suggest SO<sub>2</sub> formation in interstellar ices proceeds primarily <i>via</i> an “energetic” route involving radiolytic processes, while OCS forms as a result of “nonenergetic” processes such as atom or radical addition reactions.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1227–1242 1227–1242"},"PeriodicalIF":2.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.5c00036","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946497","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cosmic Ray Irradiation of Interstellar Ices on Sulfur-Rich Grains: A Possible Source of Sulfur-Bearing Molecules. 宇宙射线照射富硫颗粒上的星际冰:含硫分子的可能来源。
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-05-07 eCollection Date: 2025-05-15 DOI: 10.1021/acsearthspacechem.5c00036
Duncan V Mifsud, Zuzana Kaňuchová, Olivier Auriacombe, Péter Herczku, Danna Qasim, Sándor T S Kovács, Richárd Rácz, Béla Sulik, Zoltán Juhász, István Rajta, István Vajda, Sándor Biri, Robert W McCullough, Sergio Ioppolo, Ujjwal Raut, Nigel J Mason
{"title":"Cosmic Ray Irradiation of Interstellar Ices on Sulfur-Rich Grains: A Possible Source of Sulfur-Bearing Molecules.","authors":"Duncan V Mifsud, Zuzana Kaňuchová, Olivier Auriacombe, Péter Herczku, Danna Qasim, Sándor T S Kovács, Richárd Rácz, Béla Sulik, Zoltán Juhász, István Rajta, István Vajda, Sándor Biri, Robert W McCullough, Sergio Ioppolo, Ujjwal Raut, Nigel J Mason","doi":"10.1021/acsearthspacechem.5c00036","DOIUrl":"10.1021/acsearthspacechem.5c00036","url":null,"abstract":"<p><p>The major reservoir of sulfur in dense interstellar clouds is still largely unknown, although a growing body of evidence suggests that it may exist in a refractory form (i.e., as minerals or allotropes of the element). Therefore, it is possible that the irradiation of sulfur-free interstellar ices on top of sulfur-rich refractory grain components by cosmic rays or stellar winds may result in the formation of simple inorganic sulfur molecules that could be readily detected by ground- or space-borne telescopes. In this study, we have irradiated neat ices of O<sub>2</sub>, CO, CO<sub>2</sub>, and H<sub>2</sub>O on top of layers of allotropic sulfur at 20 K using 1 MeV He<sup>+</sup> ions as a mimic of space radiation. Experiments with CO<sub>2</sub> and H<sub>2</sub>O ices were also repeated at 70 K to provide data obtained under conditions more relevant to icy bodies in the outer solar system for comparative purposes. We have found qualitative mid-infrared spectroscopic evidence for the synthesis of SO<sub>2</sub>, CS<sub>2</sub>, OCS, and H<sub>2</sub>SO<sub>4</sub> hydrates, but not H<sub>2</sub>S, in our experiments and have quantified the efficiency of their formation by calculating the <i>G</i>-value (i.e., the number of molecules formed per 100 eV of energy deposited) for each ice-refractory system. Overall, SO<sub>2</sub> and CS<sub>2</sub> are the most commonly observed products in our experiments, although the highest <i>G</i>-value was that for H<sub>2</sub>SO<sub>4</sub> hydrates formed as a result of the irradiation of H<sub>2</sub>O ice on top of sulfur at 70 K. An important outcome of our study is that our experimental results are consistent with recent observational surveys that suggest SO<sub>2</sub> formation in interstellar ices proceeds primarily <i>via</i> an \"energetic\" route involving radiolytic processes, while OCS forms as a result of \"nonenergetic\" processes such as atom or radical addition reactions.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1227-1242"},"PeriodicalIF":2.9,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12086964/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144109016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Carbon and Nitrogen Fractionation in the Formation of Plant-Derived Iron Mineral-Associated Organic Matter 植物源铁矿伴生有机质形成过程中的碳氮分馏
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-05-06 DOI: 10.1021/acsearthspacechem.4c0040010.1021/acsearthspacechem.4c00400
Fei Chen, Zhe Li, Xiaofeng Cui, Leyun Wang, Erdeng Du, Xiang Liu and Miao Li*, 
{"title":"Carbon and Nitrogen Fractionation in the Formation of Plant-Derived Iron Mineral-Associated Organic Matter","authors":"Fei Chen,&nbsp;Zhe Li,&nbsp;Xiaofeng Cui,&nbsp;Leyun Wang,&nbsp;Erdeng Du,&nbsp;Xiang Liu and Miao Li*,&nbsp;","doi":"10.1021/acsearthspacechem.4c0040010.1021/acsearthspacechem.4c00400","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00400https://doi.org/10.1021/acsearthspacechem.4c00400","url":null,"abstract":"<p >Molecular fractionation during iron mineral-associated organic matter (Fe-MAOM) formation determines the turnover of various organic components and plays a vital part in carbon (C) sequestration. Nitrogen (N) enrichment in Fe-MAOM, a key fractionation outcome, exacerbates the N limitation in soil C sequestration by restricting N bioavailability, particularly for plant-derived water-soluble organic matter (WSOM) with a high C/N ratio. Here, we investigated the C and N fractionation during plant-derived WSOM binding with ferrihydrite (Fh), a poorly crystalline Fe (oxy)hydroxide exhibiting high reactivity toward organic matter. The findings demonstrated that as the molar C/Fe ratio increased, the N enrichment degree of Fe-MAOM first increased and then plateaued. This trend, as observed in molecular-level fractionation and bound organic matter speciation, was attributed to the dominant WSOM binding mechanism shifting from Fh-organic matter (Fh-OM) interactions (high selectivity) to organic matter-organic matter (OM-OM) interactions (lower selectivity) as the C/Fe ratio increased. N enrichment originated from the direct binding of proteins via Fh-OM interactions and the indirect binding of amino acids via OM-OM interactions. While coprecipitation and adsorption processes exhibit similar N enrichment degrees, the former sequesters more N via Fe(III) complexation and precipitation and would further restrict N bioavailability. These findings enhance our understanding of the N limitation in soil C sequestration and contribute to refining the models of coupled C and N biogeochemical cycling.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1070–1081 1070–1081"},"PeriodicalIF":2.9,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946450","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modeling Tropospheric Aqueous Interfacial Chemistry and Bulk Interaction with CAPRAM-HET2.0 用CAPRAM-HET2.0模拟对流层水界面化学和体相互作用
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-05-05 DOI: 10.1021/acsearthspacechem.5c0003110.1021/acsearthspacechem.5c00031
Marvel B. E. Aiyuk, Erik H. Hoffmann, Andreas Tilgner, Ralf Wolke and Hartmut Herrmann*, 
{"title":"Modeling Tropospheric Aqueous Interfacial Chemistry and Bulk Interaction with CAPRAM-HET2.0","authors":"Marvel B. E. Aiyuk,&nbsp;Erik H. Hoffmann,&nbsp;Andreas Tilgner,&nbsp;Ralf Wolke and Hartmut Herrmann*,&nbsp;","doi":"10.1021/acsearthspacechem.5c0003110.1021/acsearthspacechem.5c00031","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00031https://doi.org/10.1021/acsearthspacechem.5c00031","url":null,"abstract":"<p >Reactions at the air–water interfaces of any aqueous tropospheric particles, such as water-containing aerosol particles, haze, fog, cloud and rain droplets, can be important for atmospheric chemistry through their specific properties, which can increase the rates for certain reactions. Such accelerations can occur through (i) increased concentrations, (ii) increased rate constants, or (iii) a combination of both. A proper process description in models remains challenging due to the lack of data for both the above issues (i), (ii), and (iii). The first challenge was overcome by deriving a relationship between bulk–interface partition coefficients and octanol–water partition coefficients. This allowed us to calculate the interfacial concentration for numerous species. Results show that less soluble species prefer the interface, while the more soluble species prefer the bulk. A developed interfacial reaction mechanism was coupled to the CAPRAM bulk mechanism and applied for model simulations with an urban scenario. The simulation results show that interfacial chemistry can influence both the gas and aqueous composition, and systems with important effects are identified. Among the gas-phase species, HONO and the halogen compounds (Cl<sub>2</sub>, Br<sub>2</sub>, and I<sub>2</sub>) were most affected. A HONO concentration increase by up to 348% was modeled during cloud periods. Despite a decrease of Cl<sub>2</sub> modeled on average, a daytime in-cloud concentration increase by 62% was modeled, mainly due to the interfacial reaction of HOCl with Cl<sup>–</sup> and H<sup>+</sup>. Moreover, the modeling demonstrated that less soluble organic species can get more efficiently oxidized at the interface due to their stronger enrichment. This enables higher concentrations of some oxidized organic compounds, such as lactic acid (+18%), indicating that interfacial chemistry can support aqSOA formation.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1204–1216 1204–1216"},"PeriodicalIF":2.9,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.5c00031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143950371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exploring Anthracene in Laser-Induced Carbon Plasma Studies with Long-Wave Infrared Laser-Induced Breakdown Spectroscopy for Understanding Carbon Microstructure Formation in Space 利用长波红外激光诱导击穿光谱技术探索激光诱导碳等离子体中的蒽
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-30 DOI: 10.1021/acsearthspacechem.5c0000110.1021/acsearthspacechem.5c00001
Clayton S.-C. Yang*, Vincent J. Esposito, Laszlo Nemes, Feng Jin, Sudhir Trivedi, Uwe Hommerich and Alan C. Samuels, 
{"title":"Exploring Anthracene in Laser-Induced Carbon Plasma Studies with Long-Wave Infrared Laser-Induced Breakdown Spectroscopy for Understanding Carbon Microstructure Formation in Space","authors":"Clayton S.-C. Yang*,&nbsp;Vincent J. Esposito,&nbsp;Laszlo Nemes,&nbsp;Feng Jin,&nbsp;Sudhir Trivedi,&nbsp;Uwe Hommerich and Alan C. Samuels,&nbsp;","doi":"10.1021/acsearthspacechem.5c0000110.1021/acsearthspacechem.5c00001","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00001https://doi.org/10.1021/acsearthspacechem.5c00001","url":null,"abstract":"<p >Long-wave infrared laser-induced breakdown spectroscopy (LWIR LIBS) of anthracene, a representative polycyclic aromatic hydrocarbon, under high-energy plasma conditions, combined with harmonic and anharmonic emission spectral simulations and HITRAN-based analyses, uncovers potential pathways of molecular fragmentation, recombination, and intermediate formation, identifying small hydrocarbons (e.g., CH<sub>4</sub> and C<sub>2</sub>H<sub>2</sub>) and aromatic compounds (e.g., benzene and naphthalene). The experimental setup facilitated the simultaneous acquisition of UV/vis/NIR and LWIR spectra, offering a comprehensive analysis of molecular dynamics in a controlled plasma environment. Key findings demonstrate the influence of carrier gases, with argon inducing extensive fragmentation and helium maintaining the structural integrity of anthracene. Intriguingly, emission features at 6.98 and 8.3 μm suggest the possible presence of transient fullerenes, warranting further investigation. This study highlights the utility of LWIR LIBS for elucidating the fundamental mechanisms of cosmic carbon synthesis, offering insights into interstellar dust formation, planetary surface chemistry, and the pathways of prebiotic organic evolution. Future integration with mass spectrometry is proposed to enhance molecular identification and expand the understanding of plasma-induced carbon chemistry.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1094–1106 1094–1106"},"PeriodicalIF":2.9,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
In Situ Monitoring of the Aging of Mineral Particles by Methylglyoxal Using Infrared Spectroscopy. Part I: Unraveling Uptake under Dry Conditions 甲基乙二醛红外光谱原位监测矿物颗粒老化。第一部分:干燥条件下的分解吸收
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-30 DOI: 10.1021/acsearthspacechem.5c0003810.1021/acsearthspacechem.5c00038
Anaïs Lostier*, Frederic Thevenet and Manolis N. Romanias, 
{"title":"In Situ Monitoring of the Aging of Mineral Particles by Methylglyoxal Using Infrared Spectroscopy. Part I: Unraveling Uptake under Dry Conditions","authors":"Anaïs Lostier*,&nbsp;Frederic Thevenet and Manolis N. Romanias,&nbsp;","doi":"10.1021/acsearthspacechem.5c0003810.1021/acsearthspacechem.5c00038","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00038https://doi.org/10.1021/acsearthspacechem.5c00038","url":null,"abstract":"<p >This study examines the aging process of atmospheric mineral particles through their interaction with methylglyoxal (MGL) under dry conditions, employing diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The mineral samples used are natural dusts from the Sahara (M’Bour) and Gobi deserts, along with their principal constituents, quartz (SiO<sub>2</sub>) and calcite (CaCO<sub>3</sub>). DRIFTS spectra indicate that MGL uptake on SiO<sub>2</sub>, CaCO<sub>3</sub>, M’Bour, and Gobi dust surfaces is influenced by both reactive and nonreactive pathways. Reactive uptake results in the formation of carboxylic acids, enols, or oligomers, contributing to secondary organic aerosol formation. MGL is preferentially taken up by OH sites. Although uptake on CaCO<sub>3</sub> and Gobi dust is irreversible, M’Bour dust exhibits partial reversibility (∼25%). These findings highlight the significant role of mineral dust in atmospheric chemical processes, necessitating further investigations to evaluate the influence of humidity on uptake mechanisms and secondary organic aerosol formation.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1243–1255 1243–1255"},"PeriodicalIF":2.9,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Deciphering the Complexity in the Rotational Spectrum of Deuterated Ethylene Glycol. 解译氘化乙二醇旋转光谱的复杂性。
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-29 eCollection Date: 2025-05-15 DOI: 10.1021/acsearthspacechem.5c00067
Jordan A Claus, Mattia Melosso, Agathe Maillard, Luca Bizzocchi, Vincenzo Barone, Cristina Puzzarini
{"title":"Deciphering the Complexity in the Rotational Spectrum of Deuterated Ethylene Glycol.","authors":"Jordan A Claus, Mattia Melosso, Agathe Maillard, Luca Bizzocchi, Vincenzo Barone, Cristina Puzzarini","doi":"10.1021/acsearthspacechem.5c00067","DOIUrl":"10.1021/acsearthspacechem.5c00067","url":null,"abstract":"<p><p>Ethylene glycol (CH<sub>2</sub>OH-CH<sub>2</sub>OH) is an abundant \"complex organic molecule\" (COM) detected in different astronomical objects, but the steps of its interstellar synthesis are not yet fully understood. In this respect, the observation of deuterated isotopologues could offer insights into its formation mechanism as well as into its chemical evolution in space. Such observations, however, require detailed spectroscopic knowledge of their rotational features. Here, we present an extensive analysis of the rotational spectrum of oxygen-deuterated ethylene glycol, including the singly and doubly deuterated forms. The new measurements, carried out between 75 and 450 GHz, significantly expand the spectroscopic knowledge of the <i>aGg</i>' conformers of the CH<sub>2</sub>OH-CH<sub>2</sub>OD, CH<sub>2</sub>OD-CH<sub>2</sub>OH, and CH<sub>2</sub>OD-CH<sub>2</sub>OD species. We also report, for the first time, the laboratory identification of the <i>gGg</i>' conformers of the two mono-deuterated species. Our results reveal previously unobserved perturbations arising from the interaction between CH<sub>2</sub>OH-CH<sub>2</sub>OD and CH<sub>2</sub>OD-CH<sub>2</sub>OH, which has been modeled by including Coriolis coupling and Fermi constants in the Hamiltonian and allowed the accurate determination of the energy difference among them. Additionally, we observed significant anomalies in the spectrum of the doubly deuterated species, which seem to be caused by accidental degeneracies between the levels of the two tunneling substates. Despite the complexity and difficulties, the improved spectroscopic parameters derived from our analyses provide a solid base for future interstellar searches of deuterated ethylene glycol, enhancing our understanding of the evolution of COMs in the interstellar medium.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1267-1276"},"PeriodicalIF":2.9,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12086960/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144109025","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Deciphering the Complexity in the Rotational Spectrum of Deuterated Ethylene Glycol 解译氘化乙二醇旋转光谱的复杂性
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-29 DOI: 10.1021/acsearthspacechem.5c0006710.1021/acsearthspacechem.5c00067
Jordan A. Claus, Mattia Melosso*, Agathe Maillard, Luca Bizzocchi, Vincenzo Barone and Cristina Puzzarini, 
{"title":"Deciphering the Complexity in the Rotational Spectrum of Deuterated Ethylene Glycol","authors":"Jordan A. Claus,&nbsp;Mattia Melosso*,&nbsp;Agathe Maillard,&nbsp;Luca Bizzocchi,&nbsp;Vincenzo Barone and Cristina Puzzarini,&nbsp;","doi":"10.1021/acsearthspacechem.5c0006710.1021/acsearthspacechem.5c00067","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00067https://doi.org/10.1021/acsearthspacechem.5c00067","url":null,"abstract":"<p >Ethylene glycol (CH<sub>2</sub>OH–CH<sub>2</sub>OH) is an abundant “complex organic molecule” (COM) detected in different astronomical objects, but the steps of its interstellar synthesis are not yet fully understood. In this respect, the observation of deuterated isotopologues could offer insights into its formation mechanism as well as into its chemical evolution in space. Such observations, however, require detailed spectroscopic knowledge of their rotational features. Here, we present an extensive analysis of the rotational spectrum of oxygen-deuterated ethylene glycol, including the singly and doubly deuterated forms. The new measurements, carried out between 75 and 450 GHz, significantly expand the spectroscopic knowledge of the <i>aGg</i>′ conformers of the CH<sub>2</sub>OH–CH<sub>2</sub>OD, CH<sub>2</sub>OD–CH<sub>2</sub>OH, and CH<sub>2</sub>OD–CH<sub>2</sub>OD species. We also report, for the first time, the laboratory identification of the <i>gGg</i>′ conformers of the two mono-deuterated species. Our results reveal previously unobserved perturbations arising from the interaction between CH<sub>2</sub>OH–CH<sub>2</sub>OD and CH<sub>2</sub>OD–CH<sub>2</sub>OH, which has been modeled by including Coriolis coupling and Fermi constants in the Hamiltonian and allowed the accurate determination of the energy difference among them. Additionally, we observed significant anomalies in the spectrum of the doubly deuterated species, which seem to be caused by accidental degeneracies between the levels of the two tunneling substates. Despite the complexity and difficulties, the improved spectroscopic parameters derived from our analyses provide a solid base for future interstellar searches of deuterated ethylene glycol, enhancing our understanding of the evolution of COMs in the interstellar medium.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1267–1276 1267–1276"},"PeriodicalIF":2.9,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.5c00067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Isotopic Composition of the Noble Gases and of Some Other Elements in the Sun: A Review and a Discussion of Open Questions 太阳中惰性气体和其他元素的同位素组成:评述和若干悬而未决问题的讨论
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-29 DOI: 10.1021/acsearthspacechem.5c0000910.1021/acsearthspacechem.5c00009
Rainer Wieler*,  and , Donald S. Burnett, 
{"title":"Isotopic Composition of the Noble Gases and of Some Other Elements in the Sun: A Review and a Discussion of Open Questions","authors":"Rainer Wieler*,&nbsp; and ,&nbsp;Donald S. Burnett,&nbsp;","doi":"10.1021/acsearthspacechem.5c0000910.1021/acsearthspacechem.5c00009","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00009https://doi.org/10.1021/acsearthspacechem.5c00009","url":null,"abstract":"<p >The isotopic composition of highly volatile elements (noble gases, carbon, nitrogen, and oxygen) in the solar accretion disk is largely unconstrained by meteorite data and must be inferred independently. The best proxy is the present-day Sun, whose isotopic composition is most precisely obtained in the solar wind. Measurements from NASA’s Genesis mission provide high-precision isotopic data for most ultravolatile elements. We review these data for the noble gases, O and N in Genesis collectors, which sampled bulk solar wind for 2.3 years, as well as He, Ne, and Ar from solar wind in different velocity ranges. To obtain accurate isotopic compositions for the Sun, solar wind data require corrections for gravitational element settling in the Sun’s Outer Convective Zone (OCZ), and, more importantly, for isotopic fractionation upon formation and acceleration of the solar wind. Although a comprehensive theory to explain this fractionation is lacking, a model known as inefficient Coulomb drag (ICD) provides a plausible match to existing data. We discuss the evidence supporting this conclusion. A future determination of the carbon composition in solar wind might provide a further check. While ICD appears to reasonably characterize the isotopic fractionation between OCZ and solar wind for elements with masses up to about Ar, it may overestimate the fractionation of Kr and Xe. Precise analyses of the isotopic composition of Kr and Xe in Genesis collectors that sampled high-speed and low-speed solar wind might resolve this key question for the isotope cosmochemistry of xenon and krypton.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1142–1151 1142–1151"},"PeriodicalIF":2.9,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Impact of Biomass Burning on Organic Carbon and PM2.5 Concentrations in South Korea: Comparison between Urban and Rural Areas 生物质燃烧对韩国有机碳和PM2.5浓度的影响:城乡比较
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2025-04-28 DOI: 10.1021/acsearthspacechem.5c0003910.1021/acsearthspacechem.5c00039
Jayant Nirmalkar, Ji Yi Lee, Kwangyul Lee, Joonyoung Ahn and Mijung Song*, 
{"title":"Impact of Biomass Burning on Organic Carbon and PM2.5 Concentrations in South Korea: Comparison between Urban and Rural Areas","authors":"Jayant Nirmalkar,&nbsp;Ji Yi Lee,&nbsp;Kwangyul Lee,&nbsp;Joonyoung Ahn and Mijung Song*,&nbsp;","doi":"10.1021/acsearthspacechem.5c0003910.1021/acsearthspacechem.5c00039","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00039https://doi.org/10.1021/acsearthspacechem.5c00039","url":null,"abstract":"<p >Biomass burning (BB) in Northeast Asia significantly affects air quality. However, its contribution to atmospheric particulate matter (PM<sub>2.5</sub>) and organic carbon (OC) has rarely been studied. Atmospheric PM<sub>2.5</sub> samples were collected using preheated quartz filters from December 15, 2020, to January 14, 2021, during the winter period, from Seoul and Seosan, Republic of Korea. BB tracers, including levoglucosan and mannosan, were quantified from filter sample extracts using gas chromatography–mass spectrometry (GC-MS) analysis, and potassium ions (K<sup>+</sup>) were measured using an online aerosol inorganic monitor (AIM). Concurrently, PM<sub>2.5</sub> mass, OC, and ions were measured. The type of BB, such as hardwood, softwood, crops, grass, duff, and leaves, was identified using the levoglucosan/mannosan and levoglucosan/K<sup>+</sup>-BB ratios. The concentration of OC attributed to BB (OC-BB) was calculated by multiplying the measured levoglucosan concentration by the optimized OC/levoglucosan ratio derived from the source samples. The optimum OC/levoglucosan ratio was calculated using regression analysis between OC from non-BB sources (OC-non-BB) and levoglucosan measured at the site. Softwood was identified as the primary BB source at both sites. The optimal OC/levoglucosan ratios were 21.4 and 13.1 in Seoul and Seosan, respectively. The contribution of OC-BB to the total OC was significantly higher in Seosan (58 ± 18% and 60 ± 24%) than in Seoul (47 ± 10% and 27 ± 17%) during the winter and spring periods, respectively. The data obtained in this study are valuable for the global scientific community in estimating OC-BB contributions, which can be applied to other locations, different particle sizes, and BB types, providing a framework for assessing and mitigating biomass burning activities.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 5","pages":"1256–1266 1256–1266"},"PeriodicalIF":2.9,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946393","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信