ACS Earth and Space Chemistry最新文献

{"title":"Microsolvation of Charged PAH Clusters: Modeling Interaction of Water Aggregates with Cationic Pyrene Dimer","authors":"Héloïse Leboucher,&nbsp;Mathias Rapacioli and Aude Simon*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00099","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00099","url":null,"abstract":"<p >The interaction of polycyclic aromatic hydrocarbons (PAHs) aggregates with water plays a key role in both atmospheric and interstellar chemistry. However, its characterization at the molecular level represents experimental and theoretical challenges. In this work, we propose a detailed characterization of the potential energy surfaces (PES) of cationic pyrene dimer interacting with water molecules and clusters, Py₂⁺(H₂O)_<i>n</i> (<i>n</i> = 1–10). A dedicated PES global exploration algorithm, parallel tempering Monte Carlo, combined with the density functional tight-binding configuration interaction potential, was employed with further refinement at the density functional theory level. Structural patterns were identified, and their relative stabilities were determined. For small clusters, side isomers are found to be the most stable, while face isomers become competitive for larger sizes. Analysis of cohesive energies, relative stabilities, and evaporation energies highlights the subtle effects of noncovalent interactions and reveals size-dependent patterns. Infrared spectral signatures are predicted in the spectral region corresponding to interstellar aromatic infrared bands (AIBs), including modifications of the C–H stretch band with a new red-shifted component, and the appearance of new features in the 10–20 μm region, while the 6–10 μm range remains quite unaffected. These results provide molecular-level insight into microhydrated PAH cationic clusters that are experimentally out of reach. The obtained data are relevant for astrochemical models and the interpretation of astronomical observations, particularly in the context of James Webb Space Telescope observations.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 6","pages":"1652–1665"},"PeriodicalIF":2.6,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148268269","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}

{"title":"A Review of Molecular Simulation Techniques Applied in Microscopic Occurrence Patterns of Shale Gas","authors":"Yansong Wang,&nbsp;Yifan Gu,&nbsp;Junwei Pu,&nbsp;Lin Jiang,&nbsp;Yuqiang Jiang,&nbsp;Kun Zhang and Hu Li*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00015","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00015","url":null,"abstract":"<p >Shale gas is an unconventional hydrocarbon resource existing within the microscopic pores of shale, with a substantial fraction stored as adsorbed gas. Investigating the microscopic accumulation patterns of shale gas is critical for global shale gas exploration and development. As a new method, molecular simulation has emerged as a powerful tool to investigate the microscopic accumulation mechanisms of shale gas in nanopores. Beginning with the methodology and procedures of molecular simulation, this study first introduces the definitions of key parameters, including isosteric heat of adsorption, adsorption amount, density distribution profile, and diffusion coefficients. Subsequently, this study systematically evaluates the effects of temperature, pressure, pore morphology, pore size, gas component, and mineral composition on microscopic occurrence of shale gas. A higher temperature and lower pressure are not conducive to shale gas microscopic occurrence. Pore morphology affects shale gas microscopic occurrence at the pore scale by controlling the number and spatial distribution of adsorption layers at the microscopic scale. Shale components differ in their methane adsorption capacities. Gas competitive adsorption also influences the microscopic occurrence of shale gas. Molecular simulation elucidates the mechanism and controlling factors of adsorbed gas and free gas in shale reservoirs from the microscopic scale, and provides guidance for the optimization and efficient exploration and development of shale oil and gas “sweet spots”.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 6","pages":"1464–1478"},"PeriodicalIF":2.6,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148268431","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}

{"title":"The [3+1] Formulation of Chemical Dynamics in Curved Spacetime under an Eulerian Observer","authors":"Xingyu Zhang,&nbsp;Jinke Yu and Qingyong Meng*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00075","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00075","url":null,"abstract":"<p >Traditionally, gravity is generally considered to exert an extremely weak effect in chemistry because Newtonian gravitation is typically negligible compared to the dominant Coulomb potentials in a molecular system. In this work, we propose a primitive framework of chemical dynamics in curved spacetime through a [3 + 1] formulation. To implement this framework, the nuclear Hamiltonian operator is revised by the metric tensor of the space rather than by simply adding Newtonian gravitation in the potential energy term. For the primitive framework, the reference frames fixed on the Eulerian observers are chosen, where the absolute space and universal time viewpoint of Galileo can be adopted. This choice can be directly interfaced with the existing flat-spacetime framework, enabling us to explore the present framework for a curved spacetime. Taking spherically symmetric curved spacetime (i.e., Schwarzschild spacetime) as a numerical demonstration, we explore (1) the H + H₂ reaction dynamics, (2) the H₂ + H₂ scattering dynamics, (3) the dynamics of dissociative chemisorption of H₂O on Cu(111), (4) the spectrum band of the anthracene cation, and (5) the Berry phase in the nuclear wave function of a 98D surface scattering model. These calculations predict that (i) the reaction or scattering probability and (ii) the spectrum band decrease abruptly to zero as the spacetime curvature increases; meanwhile, the geometric phase is unaffected by the spacetime curvature. Finally, discussions on these numerical results, together with perspectives on the applications of quantum field theory to chemical dynamics in curved spacetime, are given.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 6","pages":"1613–1625"},"PeriodicalIF":2.6,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148268444","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}

{"title":"Mechanistic Insights into Environmental Aging and Reactive Nitrogen Species Generation on Dissolved Black Nitrogen and Their Contribution to Bisphenol A Photodegradation","authors":"Chaoqi Wu,&nbsp;Yuyao Zhang,&nbsp;Kaiyue Yin,&nbsp;Xinyuan Deng and Fei Lian*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00063","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00063","url":null,"abstract":"<p >Beyond dissolved black carbon (DBC), wildfires also produce substantial amounts of dissolved black nitrogen (DBN) in aquatic and soil systems; however, the activity and reactivity of DBN remain poorly understood. This study simulated environmental microbial oxidation and UV exposure using H₂O₂ oxidation and UV irradiation, respectively, and investigated their effects on the structural evolution of DBN and its subsequent photocatalytic degradation of bisphenol A (BPA). DBN was derived from nitrogen-rich biomass pyrolyzed at 350, 550, and 750 °C, respectively. The results showed that H₂O₂ oxidation increased the content of oxygen-containing groups and nitrogen oxides, as well as structural defects on DBN surfaces, more substantially than UV irradiation. H₂O₂ oxidation markedly enhanced the photodegradation of BPA by DBN, especially for DBN prepared at 350 °C. In contrast, UV-aged DBN exhibited only a modest effect on BPA photodegradation. Correlation analysis revealed that BPA removal correlated strongly with the electron-accepting capacity (EAC) of DBN (<i>R</i>² = 0.9143). The increased oxygen and nitrogen contents and the elevated EAC played dominant roles in the photodegradation of BPA by aged DBN. Nitrogen oxides promoted the generation of reactive nitrogen species (RNS), while the enhanced EAC facilitated the photoexcitation of aged DBN to form charge-separated intermediates (DBN^•+/•–), leading to hydroxyl-radical production. Both RNS and hydroxyl radicals served as the dominant free radicals, collectively oxidizing BPA and accelerating its photodegradation. This study provides novel insights into the structural transformation of DBN during environmental aging and its impact on the fate of organic pollutants.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 6","pages":"1603–1612"},"PeriodicalIF":2.6,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148268447","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}

{"title":"Guaranteed Mass-Conserving Deep Learning Model for Stiff Kinetics in Atmospheric Chemistry","authors":"Haodong Feng,&nbsp;, ,&nbsp;Yuzhong Zhang*,&nbsp;, ,&nbsp;Peiyan Hu,&nbsp;, ,&nbsp;Ruiqi Feng,&nbsp;, ,&nbsp;Yue Wang*,&nbsp;, ,&nbsp;Tailin Wu*,&nbsp;, and ,&nbsp;Dixia Fan*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00004","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00004","url":null,"abstract":"<p >Atmospheric chemistry modeling faces significant computational challenges due to stiff coupled ordinary differential equation (ODE) systems with reaction rates spanning multiple orders of magnitude. Traditional numerical solvers have been computational bottlenecks in chemical transport models (CTMs), while existing deep learning approaches suffer from mass conservation violations and catastrophic error accumulation. To overcome the above issues, we propose mass-conserving flow matching (MC-Flow), a theoretically guaranteed mass-conserving deep learning model for stiff atmospheric chemistry ODEs. MC-Flow employs generative modeling that directly predicts final states from initial conditions, bypassing intermediate transitions to eliminate error accumulation. Moreover, we theoretically derive a guaranteed mass conservation constraint and modify the training and inference procedures within the flow matching framework according to the theorem. We validate the MC-Flow on H₂O₂/OH/HO₂ system, the Verwer system, and the tropospheric CH₄–CO–NO_x–HO_x chemical system. Results demonstrate significant improvement in accuracy, both for single-step and long-term predictions with 11-fold computational speedup over numerical solvers. MC-Flow maintains guaranteed mass conservation, while comparison methods show conservation violations. The study offers a physically consistent and computationally efficient alternative to conventional numerical methods, enabling potentially an AI-driven module for atmospheric chemistry modeling with applications in air quality and climate modeling.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1320–1328"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968273","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}

{"title":"Iodine at the Aerosol–Cloud Interface: Insights from Airborne Cloud Water Measurements","authors":"Lakshmi Parakkat,&nbsp;, ,&nbsp;Mojtaba AzadiAghdam,&nbsp;, ,&nbsp;Grace Betito,&nbsp;, ,&nbsp;Rachel Braun,&nbsp;, ,&nbsp;Andrea F. Corral,&nbsp;, ,&nbsp;Ewan C. Crosbie,&nbsp;, ,&nbsp;Eva-Lou Edwards,&nbsp;, ,&nbsp;Miguel Ricardo A. Hilario,&nbsp;, ,&nbsp;Alexander B. MacDonald,&nbsp;, ,&nbsp;Ali Hossein Mardi,&nbsp;, ,&nbsp;Kayla M. Preisler,&nbsp;, ,&nbsp;Michael A. Shook,&nbsp;, ,&nbsp;Edward L. Winstead,&nbsp;, ,&nbsp;Kira Zeider,&nbsp;, ,&nbsp;Luke D. Ziemba,&nbsp;, and ,&nbsp;Armin Sorooshian*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00039","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00039","url":null,"abstract":"<p >Iodine plays a critical role in tropospheric chemistry by influencing oxidative capacity, catalyzing ozone depletion, and driving new particle formation in the marine boundary layer. However, observations of iodine in cloud water remain underexplored. This study presents a characterization of cloud water iodine concentrations from two aircraft campaigns over contrasting marine environments: Northwest Atlantic (NWA; 2020–2022) and Northeast Pacific (NEP; 2011–2016). Iodine concentrations are higher and more variable over the NEP (median = 0.013 mg L^–1, IQR = 0.014 mg L^–1) compared to the NWA (median = 0.005 mg L^–1; IQR = 0.008 mg L^–1). Over the NWA, elevated concentrations (&gt;0.020 mg L^–1) coincide with the nutrient-rich cooler side of the Gulf Stream with lower values (&lt;0.010 mg L^–1) on the oligotrophic, warmer open ocean side. Over the NEP, a decreasing offshore gradient suggests a link to ocean productivity, driven by upwelling. Principal Component Analysis reveals that iodine covaries with the species associated with marine and anthropogenic sources. Correlation analysis shows that iodine is strongly correlated with nonsea salt (NSS) SO₄^2– (0.53), MSA (0.41), and Na⁺ (0.30) for the NWA and with NO₃^– (0.51), Br^– (0.48), and oxalate (0.44) over the NEP. Machine learning modeling identified NSS SO₄^2– (NWA) and Br^– (NEP) as the most influential statistical predictors for iodine with comparable predictive performance in both regions (<i>r</i>² ≈ 0.65). These results provide an observational baseline for understanding iodine variability in cloud water and a foundation for evaluating its role in marine tropospheric chemistry and cloud processes.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1400–1417"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968283","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}

{"title":"The Reaction between Cyclopropane and the CN Radical: A Theoretical Study of Potential Astrochemical Relevance","authors":"Yeljair Monascal,&nbsp;, ,&nbsp;Vincent J. Esposito,&nbsp;, ,&nbsp;Ryan C. Fortenberry,&nbsp;, and ,&nbsp;María P. Badenes*,&nbsp;","doi":"10.1021/acsearthspacechem.5c00395","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00395","url":null,"abstract":"<p >This study presents a comprehensive theoretical investigation of the kinetics and mechanism of the <i>c</i>-C₃H₆ + CN reaction over the 10–740 K temperature range. The results show that hydrogen abstraction by the CN radical, yielding the cyclopropyl radical and hydrogen cyanide, is exothermic and proceeds through a submerged barrier, suggesting a favorable reaction pathway under interstellar conditions. The rate constants calculated at the CCSD(T)/cc-pVTZ//CCSD/cc-pVDZ level using the VTST method between 297 and 740 K agree very well with previously reported experimental data and fit the expression <i>k</i>^VTST = 2.93 × 10^–16 <i>T</i>^1.76 exp(0.05 kcal mol^–1/<i>RT</i>) cm³ molecule^–1 s^–1. Between 10 and 297 K, the temperature dependence <i>k</i> = 1.3 × 10^–11 (<i>T</i>/300)^−2.2 exp(−39.0/<i>T</i>) cm³ molecule^–1 s^–1 is obtained by combining the room temperature rate constant with two values calculated from the capture model. Additionally, anharmonic rovibrational data for cyanocyclopropane are computed and compared with the available experimental measurements. According to these findings, cyanocyclopropane emerges as a promising target for future astrochemical detection, most likely through radioastronomy due to its large dipole moment of 4.25 D.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1280–1290"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968275","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}

{"title":"Possible Interstellar Formation Routes of PN from PH3 + N(4S) & NH2 + P(4S) and Spectroscopic Characterization of the Intermediates Including HNPH","authors":"Ryan C. Fortenberry*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00031","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00031","url":null,"abstract":"<p >While the known interstellar molecule PN could be formed from reactions of atoms with diatomic hydrides, this work shows that PN may also be formed from reactions of phosphine or <i></i><math><msup><mover><mi>X</mi><mo>~</mo></mover><mn>2</mn></msup><msub><mi>B</mi><mn>1</mn></msub></math> NH₂ with nitrogen or phosphorus atoms, respectively. All of these species are known in the interstellar medium (ISM), and their reactions provide for means of producing PN by way of HNP/HPN and ³<i>A</i> HPNH. This work also shows that <i></i><math><msup><mover><mi>X</mi><mo>~</mo></mover><mn>2</mn></msup><msub><mi>B</mi><mn>1</mn></msub></math> PH₂ can arise from reactions of phosphine with atomic nitrogen under warm conditions. Additionally, the fundamental vibrational frequencies and spectroscopic constants for five of the intermediates in these reactions are provided: ¹<i>A</i>′ <i>trans</i>-HNPH, ¹<i>A</i>′ <i>cis</i>-HNPH, ³<i>A</i> HPNH, ³<i>A</i>″ PNH₂, and ³<i>A</i>″ NPH₂. Observation of any of these molecules, whether in the laboratory, or in the ISM could imply that reaction of PH₃/PH₂ or NH₂ with the right atoms could produce PN and possibly kickstart phosphorus’s role in prebiotic chemistry.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1391–1399"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968281","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}

{"title":"Micro- to Molecular-Scale Investigation of Uranium and Radium Mobility from Rare Earth Mining Residues","authors":"David Lemire,&nbsp;, ,&nbsp;Pier Lorenzo Solari,&nbsp;, ,&nbsp;Aurélie Jeanson,&nbsp;, ,&nbsp;François Orange,&nbsp;, ,&nbsp;Dominic Larivière*,&nbsp;, and ,&nbsp;Christophe Den Auwer*,&nbsp;","doi":"10.1021/acsearthspacechem.5c00358","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.5c00358","url":null,"abstract":"<p >Rare earth elements (REEs) are considered to be critical resources and play a key role in the development of advanced technologies. However, REE-bearing minerals often contain naturally occurring radioactive materials (NORMs), such as uranium and radium, which can pose radiological risks in mining operations if improperly treated. This study investigates the mobility and speciation of uranium and radium during weathering using a benchtop column model and three types of uranium sources: from the mine, from natural ore at secular equilibrium, and synthetically purified from decay products. Results indicate that radium exhibits a relatively high gradient of concentration in the leachate while uranium does not. Imaging techniques such as SEM-EDX revealed the colocalization of uranium within and on the surface of organic matter particles. Extended X-ray Absorption Fine Structure analysis suggests that uranyl species may be bound to the carboxylate complexes of the soil organic matter. These findings provide critical insights into the behavior of NORMs in REE mining environments, helping us to assess potential environmental risks.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1216–1227"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968287","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}

{"title":"Machine Learning Exploration of Binding Energy Distributions of H2O at Astrochemically Relevant Dust Grain Surfaces","authors":"Anant Vaishnav,&nbsp;, ,&nbsp;Niels M. Mikkelsen,&nbsp;, and ,&nbsp;Mie Andersen*,&nbsp;","doi":"10.1021/acsearthspacechem.6c00029","DOIUrl":"https://doi.org/10.1021/acsearthspacechem.6c00029","url":null,"abstract":"<p >Binding energies (BEs) of adsorbates on interstellar dust grains critically control adsorption, desorption, diffusion, and surface reactivity and therefore strongly influence astrochemical models of star- and planet-forming regions. While recent computational studies increasingly report full distributions of BEs rather than single representative values, these distributions are typically derived for either bare grain surfaces or thick water-ice mantles. In this work, we bridge these regimes by systematically investigating the BE distributions of water on partially and fully ice-covered dust grain surfaces. We employ machine learning interatomic potentials (MLIPs) based on graph neural networks to model water adsorption on graphene and on the Mg-terminated (010) surface of forsterite, representing carbonaceous and silicate grains, respectively. The models enable extensive sampling of adsorption sites on water clusters, monolayers, and bilayers generated under both crystalline (thermally processed) and amorphous (low temperature) growth conditions. At submonolayer coverage, the chemical nature of the underlying grain strongly affects both ice morphology and binding energies, with Mg–O interactions on silicate surfaces producing particularly deep binding sites. From monolayer coverage onward, adsorption on both substrates is dominated by hydrogen bonding within the ice, reducing the influence of the grain material. Across all coverages, amorphous ice structures systematically shift the BE distributions toward stronger binding compared to crystalline ice, introducing highly stable defect and pocket sites. These results demonstrate that BE distributions in the submonolayer-to-few-layer ice regime are broad and highly surface-dependent and provide physically motivated input for next-generation astrochemical models incorporating surface heterogeneity.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"10 5","pages":"1380–1390"},"PeriodicalIF":2.9,"publicationDate":"2026-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147968240","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}