ACS Earth and Space Chemistry最新文献

{"title":"","authors":"Marten T. Raaphorst*, Joan Enrique-Romero and Thanja Lamberts*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.5c00021","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144427920","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}

{"title":"","authors":"Jeffrey Paulo H. Perez*, A. Li Han Chan, J. Frederick W. Mosselmans and Liane G. Benning, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.5c00061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144357899","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}

{"title":"","authors":"Dilini K. Gamage, Elias Hasenecz, Glorianne P. Dorcé, Kathryn J. Mayer, Jon S. Sauer, Christopher Lee, Kimberly A. Prather and Elizabeth A. Stone*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.4c00412","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144427919","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}

{"title":"","authors":"Jeanne Caumartin, Karim Benzerara*, Robin Havas, Christophe Thomazo, Laurane Fogret, Vladimir Betancourt, Rosaluz Tavera, Béatrice Doisneau, Didier Jézéquel and Purificación López-García, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.5c00022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144427927","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}

{"title":"","authors":"Khanneh W. Fomba*, Daniel T. Quaye, Eric P. Achterberg, Eugene Marais and Hartmut Herrmann*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.4c00411","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144427932","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}

{"title":"","authors":"Bastien Duval, Juan Pablo Corella*, Maxime Enrico, Alfonso Saiz-Lopez, Carlos A. Cuevas, Jose A. Adame, Rocío Millán, Maria J. Sierra, Sylvain Bérail, Blas L. Valero-Garcés, Alberto de Diego, Mario Morellón, Javier Rodríguez-Alonso and David Amouroux*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.9,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsearthspacechem.4c00402","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144427939","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}

{"title":"Coexisting Phosphate Controls Arsenate Speciation and Partitioning during Fe(II)-Catalyzed Ferrihydrite Transformation.","authors":"Jeffrey Paulo H Perez, A Li Han Chan, J Frederick W Mosselmans, Liane G Benning","doi":"10.1021/acsearthspacechem.5c00061","DOIUrl":"10.1021/acsearthspacechem.5c00061","url":null,"abstract":"<p><p>Arsenic immobilization in soils and sediments is primarily controlled by its sorption onto or incorporation into reactive soil minerals, such as iron (oxyhydr)-oxides. However, coexisting ions (e.g., dissolved bicarbonate, phosphate, silica, and organic matter) can negatively impact the interaction of the toxic arsenate species with iron (oxy)-hydroxides. Of special note is inorganic phosphate, which is a strong competitor for sorption sites due to its analogous chemical and structural nature to inorganic arsenate. Much of our understanding of this competing nature between phosphate and arsenate focuses on the impact on mineral sorption capacities and kinetics. However, we know very little about how coexisting phosphate will alter the stability and transformation pathways of arsenate-bearing Fe (oxyhydr)-oxides. In particular, the long-term fate and behavior regarding arsenate immobilization are unknown under anoxic conditions. Here, we document, through mineral transformation reactions, the immobilization of both phosphate (P) and arsenate [As-(V)] in secondary mineral products and characterize their changing compositions during the transformations. We did this while controlling the initial P/As-(V) ratios. Our results document that, in the absence or at low P/As-(V) ratios, the initial ferrihydrite rapidly transforms to green rust sulfate (GR_SO₄ ), which further transforms into magnetite after 180 days. Meanwhile, high P/As-(V) ratios resulted in a mixture of GR_SO₄ and vivianite, with magnetite as a minor fraction. Invariably, the speciation and partitioning of As-(V) were also affected by the P/As-(V) ratio. A higher P/As-(V) ratio also led to a faster partial reduction of mineral-bound As-(V) to As-(III). The most important finding is that the initial ferrihydrite-bound As-(V) became structurally incorporated into magnetite [low P/As-(V) ratio] or vivianite [high P/As-(V) ratio] and was thus immobilized and not labile. Overall, our results highlight the influence of coexisting phosphate in controlling the toxicity and mobility in anoxic, Fe²⁺-rich subsurface settings, such as contaminated aquifers.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"1642-1653"},"PeriodicalIF":2.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12183708/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144482508","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}

{"title":"Coexisting Phosphate Controls Arsenate Speciation and Partitioning during Fe(II)-Catalyzed Ferrihydrite Transformation","authors":"Jeffrey Paulo H. Perez*,&nbsp;A. Li Han Chan,&nbsp;J. Frederick W. Mosselmans and Liane G. Benning,&nbsp;","doi":"10.1021/acsearthspacechem.5c0006110.1021/acsearthspacechem.5c00061","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00061https://doi.org/10.1021/acsearthspacechem.5c00061","url":null,"abstract":"<p >Arsenic immobilization in soils and sediments is primarily controlled by its sorption onto or incorporation into reactive soil minerals, such as iron (oxyhydr)oxides. However, coexisting ions (e.g., dissolved bicarbonate, phosphate, silica, and organic matter) can negatively impact the interaction of the toxic arsenate species with iron (oxy)hydroxides. Of special note is inorganic phosphate, which is a strong competitor for sorption sites due to its analogous chemical and structural nature to inorganic arsenate. Much of our understanding of this competing nature between phosphate and arsenate focuses on the impact on mineral sorption capacities and kinetics. However, we know very little about how coexisting phosphate will alter the stability and transformation pathways of arsenate-bearing Fe (oxyhydr)oxides. In particular, the long-term fate and behavior regarding arsenate immobilization are unknown under anoxic conditions. Here, we document, through mineral transformation reactions, the immobilization of both phosphate (P) and arsenate [As(V)] in secondary mineral products and characterize their changing compositions during the transformations. We did this while controlling the initial P/As(V) ratios. Our results document that, in the absence or at low P/As(V) ratios, the initial ferrihydrite rapidly transforms to green rust sulfate (GR_SO₄), which further transforms into magnetite after 180 days. Meanwhile, high P/As(V) ratios resulted in a mixture of GR_SO₄ and vivianite, with magnetite as a minor fraction. Invariably, the speciation and partitioning of As(V) were also affected by the P/As(V) ratio. A higher P/As(V) ratio also led to a faster partial reduction of mineral-bound As(V) to As(III). The most important finding is that the initial ferrihydrite-bound As(V) became structurally incorporated into magnetite [low P/As(V) ratio] or vivianite [high P/As(V) ratio] and was thus immobilized and not labile. Overall, our results highlight the influence of coexisting phosphate in controlling the toxicity and mobility in anoxic, Fe²⁺-rich subsurface settings, such as contaminated aquifers.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"1642–1653 1642–1653"},"PeriodicalIF":2.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.5c00061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312311","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}

{"title":"Modeling the Tropospheric Aqueous-Phase Chemistry of Photosensitizers under Wildfire-Plume and Urban Conditions with CAPRAM-PS1.0","authors":"Erik H. Hoffmann,&nbsp;Andreas Tilgner,&nbsp;Tamara Felber,&nbsp;Marvel B. E. Aiyuk,&nbsp;Thomas Schaefer and Hartmut Herrmann*,&nbsp;","doi":"10.1021/acsearthspacechem.5c0003310.1021/acsearthspacechem.5c00033","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00033https://doi.org/10.1021/acsearthspacechem.5c00033","url":null,"abstract":"<p >A detailed CAPRAM mechanism describing the sunlight-induced photosensitization chemistry is developed and applied to a chemical process model. The mechanism contains the gas–aqueous phase partitioning and further chemical processing of nine commonly investigated photosensitizers and particulate HULIS. In addition, the chemistry of secondarily formed singlet oxygen is included in a detailed manner. Overall, the newly developed mechanism module CAPRAM-PS1.0 comprises 284 processes. Performed model simulations focus on the environmental conditions of (i) a fresh smoke plume from a wildfire and (ii) an urban polluted background. The simulation revealed that the quenching of activated photosensitizers is dominated either by the organic matrix and copper under particle conditions or by oxygen under cloud conditions. The modeled average photosensitizer and ¹O₂ concentrations range between (0.007–9.5) × 10^–12 and (0.0002–1.1) × 10^–11 mol l^–1, respectively, and agree with measurements depending on the simulations. The main modeled loss of ¹O₂ is quenching by the water matrix with a 97% yield. The residual reactions are dominated by quenching through the organic matrix. The simulations indicate that effective quenching of photosensitizers and their main product ¹O₂ into the ground state inhibits the efficient production of particulate mass. Accordingly, great care should be taken not to overstate possible effects of photosensitization chemistry in atmospheric organic-containing aerosol particles. Besides and interestingly, photosensitizer chemistry is modeled to contribute up to 25% to chlorine activation, affecting the tropospheric oxidation budget.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"1593–1606 1593–1606"},"PeriodicalIF":2.9,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.5c00033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312314","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}

{"title":"Saharan and Namib Dust Phosphorus Fluxes in the North and South Atlantic Regions","authors":"Khanneh W. Fomba*,&nbsp;Daniel T. Quaye,&nbsp;Eric P. Achterberg,&nbsp;Eugene Marais and Hartmut Herrmann*,&nbsp;","doi":"10.1021/acsearthspacechem.4c0041110.1021/acsearthspacechem.4c00411","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.4c00411https://doi.org/10.1021/acsearthspacechem.4c00411","url":null,"abstract":"<p >Phosphorus (P) is essential for marine ecosystems, particularly in nutrient-poor regions of the Northeastern and Southeastern Tropical Atlantic (NETA/SETA). However, P deposition and bioavailability remain poorly understood, limiting predictions of its role in marine productivity. To address this, P speciation, including organic, inorganic, and soluble contents in aerosol particles, was analyzed over 19 months at the Cape Verde (CVAO) and Namib Desert (NDAO) Atmospheric Observatories. P concentrations at NDAO (56.1 ± 62 ng/m³) were 47% higher than those at CVAO (29.8 ± 76 ng/m³) with dominant coarse mode contents and fine-to-coarse ratios (PM_1.2/PM₁₀) of 0.42–0.57 at NDAO and 0.17–0.32 at CVAO. Phosphorus sources at both sites include mineral dust and biomass burning with additional biogenic aerosols at NDAO. Organic P made up 19% and 39% of total P at NDAO and CVAO, respectively. Soluble P was 20% more abundant at NDAO, linked to higher biomass burning source provenance and aerosol acidity, confirming previous reports that atmospheric processing enhances P solubility. P solubility was lower during Saharan and Namib dust events, indicating comparatively reduced solubility from mineral-dust sources. This first report of annual deposition fluxes from these regions reveals somewhat higher average values in the SETA (2.05 ± 2.8 μmol/m²d at NDAO) than the NETA (1.3 ± 3.4 μmol/m²d at CVAO), with pronounced differences in the austral winter months. Elevated dissolved inorganic nitrogen to dissolved inorganic P ratios at CVAO indicated a smaller contribution of atmospheric P deposition in mitigating nutrient limitation in the nearby waters. These findings offer new insights into atmospheric P solubility and fluxes, crucial for improving ocean-atmosphere models and understanding its ecological impacts in the tropical Atlantic.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"9 6","pages":"1465–1478 1465–1478"},"PeriodicalIF":2.9,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsearthspacechem.4c00411","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312471","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}