ACS Earth and Space Chemistry最新文献_第6页

Simulated Sea Level Rise in Coastal Peat Soils Stimulates Mercury Methylation 沿海泥炭土中的模拟海平面上升会刺激汞甲基化

IF 3.4 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-16 DOI: 10.1021/acsearthspacechem.4c00124

Bryce A. Cook, Benjamin D. Peterson, Jacob M. Ogorek, Sarah E. Janssen, Brett A. Poulin

{"title":"Simulated Sea Level Rise in Coastal Peat Soils Stimulates Mercury Methylation","authors":"Bryce A. Cook, Benjamin D. Peterson, Jacob M. Ogorek, Sarah E. Janssen, Brett A. Poulin","doi":"10.1021/acsearthspacechem.4c00124","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00124","url":null,"abstract":"Coastal wetlands are vulnerable to sea level rise with unknown consequences for mercury (Hg) cycling, particularly the potential for exacerbating neurotoxic methylmercury (MeHg) production and bioaccumulation in food webs. Here, the effect of sea level rise on MeHg formation in the Florida Everglades was evaluated by incubating peat cores from a freshwater wetland for 0–20 days in the laboratory at five salinity conditions (0.16–6.0 parts-per-thousand; 0.20–454 mg L–1 sulfate (SO42–)) to simulate the onset of sea level rise within coastal margins. Isotopically enriched inorganic mercury (201Hg(II)) was used to track MeHg formation and peat-porewater partitioning. In all five salinity treatments, porewaters became anoxic within 1 day and became progressively enriched in dissolved organic matter (DOM) of greater aromatic composition over the 20 days compared to ambient conditions. In the four highest salinity treatments, SO42– concentrations decreased and sulfide concentrations increased over time due to microbial dissimilatory SO42– reduction that was concurrent with 201Hg(II) methylation. Importantly, elevated salinity resulted in a greater proportion of produced Me201Hg observed in porewaters as opposed to bound to peat, interpreted to be due to the complexation of MeHg with aromatic DOM released from peat. The findings highlight the potential for enhanced production and mobilization of MeHg in coastal wetlands of the Florida Everglades due to the onset of saltwater intrusion.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142223775","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

Gamma-Ray-Induced Synthesis of Sugars in Meteorite Parent Bodies 伽马射线诱导陨石母体中糖类的合成

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-15 DOI: 10.1021/acsearthspacechem.4c0009910.1021/acsearthspacechem.4c00099

Shunpei Abe, Isao Yoda, Kensei Kobayashi and Yoko Kebukawa*,

{"title":"Gamma-Ray-Induced Synthesis of Sugars in Meteorite Parent Bodies","authors":"Shunpei Abe, Isao Yoda, Kensei Kobayashi and Yoko Kebukawa*, ","doi":"10.1021/acsearthspacechem.4c0009910.1021/acsearthspacechem.4c00099","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00099https://doi.org/10.1021/acsearthspacechem.4c00099","url":null,"abstract":"Sugars play an indispensable role for all living organisms. Given that certain sugars have been identified in carbonaceous chondrites, these compounds might have been delivered to the early Earth via meteorites. The genesis of these sugars, however, has been a subject of debate; they are considered to have either originated from UV irradiation of interstellar ice or from hydrothermal reactions within the environments of meteorite parent bodies. The parent bodies of carbonaceous chondrites contained water ice which underwent hydrothermal alteration as a result of the internal warming of these bodies. The most likely source of this heat is believed to be the decay of radioactive nuclides, such as 26Al. In our previous research, we demonstrated that gamma-ray exposure significantly enhances the synthesis of amino acids from aqueous solutions of formaldehyde, ammonia, and methanol. Nonetheless, the impact of radiation on sugar formation has not been investigated. Hence, the current study is conducted with a focus on the formation of aldose sugars through gamma-ray irradiation to such solution mixtures. Our results reveal that gamma-rays indeed promote the formation of sugars, including ribose, without the presence of a catalyst such as glycolaldehyde. Furthermore, we demonstrated that the presence of ammonia enhanced the yield of aldose sugars, although higher concentration of ammonia inhibited sugar production. Our findings suggest that gamma-rays from the decay of 26Al played a significant role in the formation of sugars during low-temperature aqueous alteration inside meteorite parent bodies.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":2.9,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.4c00099","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142273784","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

Gamma-Ray-Induced Synthesis of Sugars in Meteorite Parent Bodies 伽马射线诱导陨石母体中糖类的合成

IF 3.4 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-15 DOI: 10.1021/acsearthspacechem.4c00099

Shunpei Abe, Isao Yoda, Kensei Kobayashi, Yoko Kebukawa

{"title":"Gamma-Ray-Induced Synthesis of Sugars in Meteorite Parent Bodies","authors":"Shunpei Abe, Isao Yoda, Kensei Kobayashi, Yoko Kebukawa","doi":"10.1021/acsearthspacechem.4c00099","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00099","url":null,"abstract":"Sugars play an indispensable role for all living organisms. Given that certain sugars have been identified in carbonaceous chondrites, these compounds might have been delivered to the early Earth via meteorites. The genesis of these sugars, however, has been a subject of debate; they are considered to have either originated from UV irradiation of interstellar ice or from hydrothermal reactions within the environments of meteorite parent bodies. The parent bodies of carbonaceous chondrites contained water ice which underwent hydrothermal alteration as a result of the internal warming of these bodies. The most likely source of this heat is believed to be the decay of radioactive nuclides, such as 26Al. In our previous research, we demonstrated that gamma-ray exposure significantly enhances the synthesis of amino acids from aqueous solutions of formaldehyde, ammonia, and methanol. Nonetheless, the impact of radiation on sugar formation has not been investigated. Hence, the current study is conducted with a focus on the formation of aldose sugars through gamma-ray irradiation to such solution mixtures. Our results reveal that gamma-rays indeed promote the formation of sugars, including ribose, without the presence of a catalyst such as glycolaldehyde. Furthermore, we demonstrated that the presence of ammonia enhanced the yield of aldose sugars, although higher concentration of ammonia inhibited sugar production. Our findings suggest that gamma-rays from the decay of 26Al played a significant role in the formation of sugars during low-temperature aqueous alteration inside meteorite parent bodies.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142223777","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

Assessing Iron Complexation by Dissolved Organic Matter Using Mediated Electrochemical Oxidation 利用介导电化学氧化法评估溶解有机物对铁的络合作用

IF 3.4 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-14 DOI: 10.1021/acsearthspacechem.4c00131

Jeffrey M. Hudson, George W. Luther, III, Yu-Ping Chin

{"title":"Assessing Iron Complexation by Dissolved Organic Matter Using Mediated Electrochemical Oxidation","authors":"Jeffrey M. Hudson, George W. Luther, III, Yu-Ping Chin","doi":"10.1021/acsearthspacechem.4c00131","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00131","url":null,"abstract":"FeII is an abundant reductant in the environment that participates in numerous biogeochemical cycles and pollutant attenuation. FeII in aquatic environments can exist as a complex with dissolved organic matter (DOM), where organic ligands in DOM can modulate iron’s redox potential (EH) and henceforth reactivity as a reductant. Previous studies have assessed the reactivity of FeII-complexes using probe compounds, although these compounds are limited in their ability to profile FeII oxidation across multiple thermodynamic conditions (i.e., both pH and EH) and fail to validate the EH of Fe(II)-complexes via their direct measurement. This study elucidated the redox potentials of FeII-DOM complexes via mediated electrochemical oxidation (MEO) and assessed the extent of FeII oxidation at two different applied EH and pH regimes. Furthermore, we used a Nernstian-based model calibrated with a training set between known iron-ligand thermodynamic stability constants and their respective measured potentials to indirectly determine the stability constants of both FeII and FeIII-DOM complexes as a function of EH and pH. This work highlights the versatility of MEO as an electrochemical technique and is the first to assess stability constants of Fe-complexes with aquatic DOM isolates. We also discuss linkages between speciation modeling and redox reactivity of FeII.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142223778","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

High-Resolution Far- to Near-Infrared Anharmonic Absorption Spectra of Cyano-Substituted Polycyclic Aromatic Hydrocarbons from 300 to 6200 cm−1 300 至 6200 cm-1 范围内氰基取代多环芳香烃的高分辨率远红外至近红外谐波吸收光谱

IF 3.4 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-14 DOI: 10.1021/acsearthspacechem.4c00160

Vincent J. Esposito, Ryan C. Fortenberry, Christiaan Boersma, Louis J. Allamandola

{"title":"High-Resolution Far- to Near-Infrared Anharmonic Absorption Spectra of Cyano-Substituted Polycyclic Aromatic Hydrocarbons from 300 to 6200 cm−1","authors":"Vincent J. Esposito, Ryan C. Fortenberry, Christiaan Boersma, Louis J. Allamandola","doi":"10.1021/acsearthspacechem.4c00160","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00160","url":null,"abstract":"Cyano-substituted polycyclic aromatic hydrocarbons (CN-PAHs) may contribute to the emission detected in the 7−9 μm (1430−1100 cm−1) and 11−15 μm (900−670 cm−1) regions of astronomical IR spectra. Anharmonic quantum chemical computations of 14 CN-PAH isomers for 4 small PAHs and benzene reveal strong, broad absorption features across the entire 300−6200 cm−1 (33−1.6 μm) frequency range. In particular, when an full width at half maximum (fwhm) of 15 cm−1 is applied, the composite CN-PAH spectrum greatly overlaps with the unsubstituted-PAH spectrum across the entire 300−6200 cm−1 range besides the 2200−2500 cm−1 region that arises from the strong CN stretch fundamental of CN-PAHs and is addressed in a separate publication. At high resolution, however, the infrared absorption spectra reveal unique, identifiable features of CN-PAHs in the 700−950, 1100−1300, 2000−2500, and 3400−3600 cm−1 ranges. The in-plane and out-of-plane CH bending vibrational frequencies of CN-PAHs are shifted when comparing isomers and their unsubstituted counterparts, making their differentiation in mixed laboratory experiments possible. The overall aromatic CH stretch fundamental (2950−3200 cm−1) and first overtone (5950−6200 cm−1) regions are relatively unaffected by the cyano-substitution, with changes only to the frequency range covered by, and the intensity of, the bands. Detailed spectroscopic data on the normal mode components of each state reported herein provide the means to directly assign future laboratory spectra and to guide direct IR observations of astronomical regions with, e.g., James Webb Space Telescope (JWST).","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142223776","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

High-Resolution Far- to Near-Infrared Anharmonic Absorption Spectra of Cyano-Substituted Polycyclic Aromatic Hydrocarbons from 300 to 6200 cm−1 300 至 6200 cm-1 范围内氰基取代多环芳香烃的高分辨率远红外至近红外谐波吸收光谱

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-14 DOI: 10.1021/acsearthspacechem.4c0016010.1021/acsearthspacechem.4c00160

Vincent J. Esposito*, Ryan C. Fortenberry, Christiaan Boersma and Louis J. Allamandola,

{"title":"High-Resolution Far- to Near-Infrared Anharmonic Absorption Spectra of Cyano-Substituted Polycyclic Aromatic Hydrocarbons from 300 to 6200 cm−1","authors":"Vincent J. Esposito*, Ryan C. Fortenberry, Christiaan Boersma and Louis J. Allamandola, ","doi":"10.1021/acsearthspacechem.4c0016010.1021/acsearthspacechem.4c00160","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00160https://doi.org/10.1021/acsearthspacechem.4c00160","url":null,"abstract":"Cyano-substituted polycyclic aromatic hydrocarbons (CN-PAHs) may contribute to the emission detected in the 7−9 μm (1430−1100 cm−1) and 11−15 μm (900−670 cm−1) regions of astronomical IR spectra. Anharmonic quantum chemical computations of 14 CN-PAH isomers for 4 small PAHs and benzene reveal strong, broad absorption features across the entire 300−6200 cm−1 (33−1.6 μm) frequency range. In particular, when an full width at half maximum (fwhm) of 15 cm−1 is applied, the composite CN-PAH spectrum greatly overlaps with the unsubstituted-PAH spectrum across the entire 300−6200 cm−1 range besides the 2200−2500 cm−1 region that arises from the strong CN stretch fundamental of CN-PAHs and is addressed in a separate publication. At high resolution, however, the infrared absorption spectra reveal unique, identifiable features of CN-PAHs in the 700−950, 1100−1300, 2000−2500, and 3400−3600 cm−1 ranges. The in-plane and out-of-plane CH bending vibrational frequencies of CN-PAHs are shifted when comparing isomers and their unsubstituted counterparts, making their differentiation in mixed laboratory experiments possible. The overall aromatic CH stretch fundamental (2950−3200 cm−1) and first overtone (5950−6200 cm−1) regions are relatively unaffected by the cyano-substitution, with changes only to the frequency range covered by, and the intensity of, the bands. Detailed spectroscopic data on the normal mode components of each state reported herein provide the means to directly assign future laboratory spectra and to guide direct IR observations of astronomical regions with, e.g., James Webb Space Telescope (JWST).","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":2.9,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142273755","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

Assessing Iron Complexation by Dissolved Organic Matter Using Mediated Electrochemical Oxidation 利用介导电化学氧化法评估溶解有机物对铁的络合作用

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-14 DOI: 10.1021/acsearthspacechem.4c0013110.1021/acsearthspacechem.4c00131

Jeffrey M. Hudson*, George W. Luther III and Yu-Ping Chin,

{"title":"Assessing Iron Complexation by Dissolved Organic Matter Using Mediated Electrochemical Oxidation","authors":"Jeffrey M. Hudson*, George W. Luther III and Yu-Ping Chin, ","doi":"10.1021/acsearthspacechem.4c0013110.1021/acsearthspacechem.4c00131","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00131https://doi.org/10.1021/acsearthspacechem.4c00131","url":null,"abstract":"FeII is an abundant reductant in the environment that participates in numerous biogeochemical cycles and pollutant attenuation. FeII in aquatic environments can exist as a complex with dissolved organic matter (DOM), where organic ligands in DOM can modulate iron’s redox potential (EH) and henceforth reactivity as a reductant. Previous studies have assessed the reactivity of FeII-complexes using probe compounds, although these compounds are limited in their ability to profile FeII oxidation across multiple thermodynamic conditions (i.e., both pH and EH) and fail to validate the EH of Fe(II)-complexes via their direct measurement. This study elucidated the redox potentials of FeII-DOM complexes via mediated electrochemical oxidation (MEO) and assessed the extent of FeII oxidation at two different applied EH and pH regimes. Furthermore, we used a Nernstian-based model calibrated with a training set between known iron-ligand thermodynamic stability constants and their respective measured potentials to indirectly determine the stability constants of both FeII and FeIII-DOM complexes as a function of EH and pH. This work highlights the versatility of MEO as an electrochemical technique and is the first to assess stability constants of Fe-complexes with aquatic DOM isolates. We also discuss linkages between speciation modeling and redox reactivity of FeII.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":2.9,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142270009","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

A Network Approach for the Accurate Characterization of Water Lines Observable in Astronomical Masers and Extragalactic Environments 准确描述天文增量器和银河系外环境中可观测到的水线的网络方法

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-09 DOI: 10.1021/acsearthspacechem.4c00161

W. Ubachs, A. Császár, M. Diouf, F. Cozijn, Roland Tóbiás

引用次数: 0

Reactant Discovery with an Ab Initio Nanoreactor: Exploration of Astrophysical N-Heterocycle Precursors and Formation Pathways 利用 Ab Initio 纳米反应器发现反应物：探索天体物理 N-杂环前体和形成途径

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-09 DOI: 10.1021/acsearthspacechem.4c00120

Sommer L. Johansen, Heejune Park, Lee-Ping Wang, Kyle N Crabtree

引用次数: 0

Vacuum Ultraviolet Photoionization of Methane-Water Clusters Leads to Methanol Formation 甲烷-水簇的真空紫外光电离导致甲醇的形成

IF 2.9 3区化学

ACS Earth and Space Chemistry Pub Date : 2024-08-09 DOI: 10.1021/acsearthspacechem.4c0015110.1021/acsearthspacechem.4c00151

Nureshan Dias, Alexander K. Lemmens, Anna Wannenmacher and Musahid Ahmed*,

{"title":"Vacuum Ultraviolet Photoionization of Methane-Water Clusters Leads to Methanol Formation","authors":"Nureshan Dias, Alexander K. Lemmens, Anna Wannenmacher and Musahid Ahmed*, ","doi":"10.1021/acsearthspacechem.4c0015110.1021/acsearthspacechem.4c00151","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00151https://doi.org/10.1021/acsearthspacechem.4c00151","url":null,"abstract":"We report on the photoionization of a series of small methane-water mixed clusters generated in a supersonic jet expansion. The resulting clusters are investigated by synchrotron-based single photon vacuum ultraviolet (VUV) ionization coupled with reflectron time-of-flight mass spectrometry. Pure methane clusters (CH4)n+ and protonated water clusters (WnH)+ dominate the mass spectra, however with judicious control of backing pressure and mixing ratio, mixed methane-water clusters are generated. We gain unique insights into the underlying dynamics and chemistry of methane and mixed methane-water clusters through the analysis of fragment mass spectra, and photoionization intensity curves, which provide appearance energies, which are then compared to theoretically calculated ionization energies. In particular, we provide experimental evidence of the formation of methanol upon photoionization of the mixed clusters under cold conditions, which is directly relevant to astrochemistry.","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":null,"pages":null},"PeriodicalIF":2.9,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142270022","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