6 research outputs found
Computational Supporting Information for Methane Adsorption on Heteroatom-Modified Maquettes of Porous Carbon Surfaces
No full textThis dataset is an extensive computational supporting information for the first manuscript of a series of reports from the collaborative work of the carbon materials laboratory of Prof. Nicholas Stadie and the computational laboratory of Prof. Robert Szilagyi at Montana State University. The dataset provide atomic-scale insights into the structure and properties of amorphous carbon materials for reversible gas storage applications. The current report is focused on modeling methane adsorption on zeolite-templated carbon through invoking the concepts of maquettes: simplified models with essential functionalities preserved of the real system. We employed a converging series of explicitly correlated MO theory and density functional theory.
The theoretical approach employed is based on our previous publications
Ellis E., MacHale L.T., Szilagyi R.K., DuBois J.L.: How Chemical Environment Activates Anthralin and Molecular Oxygen for Direct Reaction Journal of Organic Chemistry, 2020, 85(2), 1315–1321 DOI: 10.1021/acs.joc.9b03133 and
Poovathingal S.J., Minton T.K., Szilagyi R.K.: Systematic evaluation of density functionals for electronic and geometric Structures: Chemical speciation of mononuclear Ru-Cl-H-PR3 complexes Journal of Physical Chemistry, Part A. 2019, 123(1), 343–358 DOI: 10.1021/acs.jpca.8b03216 .
The level of theories considered here are consistent with an earlier study that was carried out independent from our focus
Nishimura Y., Tsuneda T., Sato T., Katouda M., Irle S.: Quantum chemical estimation of acetone physisorption on graphene using combined basis set and size extrapolation schemes. Journal of Physical Chemistry C 2017, 121(16), 8999–9010 DOI: 10.1021/acs.jpcc.6b13002.
Moreover, key experimental data are taken from
Stadie N.P., Murialdo M., Ahn C.C., Fultz B.: Unusual Entropy of Adsorbed Methane on Zeolite-Templated Carbon Journal of Physical Chemistry C, 2015, 119(47), 26409-26421 DOI: 10.1021/acs.jpcc.5b05021.
In addition to a comprehensive evaluation of the methane adsorption on pure-carbon maquette surface, we extended the adsorption studies to B- and N-doped adsorbents. We found consistent preference for N-doped materials for methane storage. In addition to discussing energy differences and structural variations as a function of the nature of dopant, we uncovered details of the electronic structure of methane interactions and its variability along the series of C, B, and N. The predicted heat of adsorption values are now informing on-going experimental synthetic work in the Stadie laboratory toward the optimization of gas storage materials.
The results reported in the manuscripts stimulate extension of our work to larger maquettes of porous carbon surfaces with synthetically relevant functional groups, alternative ring sizes, curvature, and other heteroatom substitutional dopants. An additional notable merit is our effort to provide a clear thermodynamic connection among microscopic and macroscopic observables related to physical properties of gas storage materials and interfaces.R.R., E.T., and N.S. are supported by the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Hydrogen and Fuel Cell Technologies and Vehicle Technologies Offices (DE-EE0008815). S.I. acknowledges support for the analysis of theoretical results by the U.S. Department of Energy's Office of Fossil Energy (FE). N.S. acknowledges the donors of the American Chemical Society Petroleum Research Fund for partial support of this research. R.R. is thankful for the support by the MSU Undergraduate Scholars Program. We are also grateful for resources provided by the Extreme Science and Engineering Discovery Environment (XSEDE), supported by National Science Foundation grant ACI-1548562.113 Part of the computations were carried out using the Hyalite High Performance Computing System, operated and supported by the University Information Technology Research Cyberinfrastructure at Montana State University
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No full textMethane Adsorption on Heteroatom-Modified Maquettes of Porous Carbon Surfaces
No full text
Experimental studies and theoretical models presently disagree on methane adsorption
energetics on carbon materials that include crystalline graphene-like structures to amorphous
materials with or without significant edge structure. However, this information is critical for the
rational design and optimization of the structure and composition of adsorbents for natural gas
storage. The delicate nature of the interactions inherent to methane physisorption, such as
dispersion interactions, polarization of both the adsorbent and the adsorbate, interplay between H-
bonding and tetrel bonding, and induced dipole/Coulomb interactions, requires computational
treatment at the highest possible level of theory while remaining non-prohibitive in terms of
computational cost. In this study, we employ the smallest reasonable computational model, a
maquette, of porous carbon surfaces with a central atomic binding site for substitution. The most
accurate predictions of the methane adsorption energetics were achieved by electron-correlated
molecular orbital theory (CCSD(T)) and hybrid density functional theory (MN15) calculations, both
employing a saturated all-electron basis set. The characteristic geometry of methane adsorption on
a carbon surface was likened to a “lander” position over the ring centers of the adsorbent. This
adsorbate/adsorbent arrangement arises due to bonding interactions of the adsorbent π-system
with the proximal H–C bonds of methane, in addition to tetrel bonding between the antibonding
orbital of the distal C–H bond and the central atom of the maquette (C, B, or N). The polarization of
the electron density as well as structural deformations in both the adsorbate and adsorbent
molecules clearly indicate a ~3 kJ mol-1 preference for methane binding on the N-substituted
maquette. In this study, the B-substituted maquette showed a comparable or lower binding energy
than the unsubstituted, pure C model, depending on the level of theory employed. The calculated
thermodynamic results indicate an unambiguous guiding strategy toward incorporating electron-
enriched substitutions (e.g., N) in carbon materials as a way to increase methane storage capacity
over electron deficient (e.g., B) modifications. The thermochemical calculation methodologies were
critically evaluated in order to establish a conceptual agreement between the experimental
isosteric heat of adsorption and the binding enthalpies/free energies from statistical
thermodynamics principles.
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Endorsement of artificial intelligence guidelines across leading obstetrics and gynecology journals: A preliminary cross-sectional analysis
No full textBackground: Artificial intelligence (AI) is transforming research in Obstetrics and Gynecology by advancing data analysis, facilitating systematic reviews, and enhancing clinical applications. However, its adoption raises concerns related to transparency, ethical considerations, and reproducibility. This study investigates how leading Obstetrics and Gynecology journals address these concerns and opportunities through their author instructions and editorial policies.Methods: A cross-sectional analysis was conducted on the top 100 peer-reviewed Obstetrics and Gynecology journals, ranked by the 2023 SCImago SJR indicator. Information was collected from each journal's "Instructions for Authors" to assess AI-related policies, including specific guidelines for reporting AI use, authorship criteria, and the role of AI in manuscript development and image creation. Correlation analyses were used to explore the relationship between AI-related policies and the journals’ characteristics.Results: Among the 100 journals reviewed, 92% included guidance on AI usage in their author instructions. Most journals prohibited AI authorship while mandating disclosure of AI involvement in manuscript submissions. While 14% of the journals allowed AI-generated content, only 7% permitted AIgenerated images. Journals with higher impact factors were more likely to have detailed AI policies, although there were notable gaps in standardization and clarity.Conclusion: Although many Obstetrics and Gynecology journals recognize the growing influence of AI in research, few have implemented specific AI reporting guidelines (RGs), limiting the consistency and transparency of AI usage. We advocate for the development of robust and standardized guidelines to ensure that research remains ethical, reproducible, and of high quality in this new era of AI innovation
Configuraciones de las imágenes de las enfermedades mentales en la serie animada BoJack Horseman
No full textEsta investigación identifica y sugiere relaciones entre la enfermedad mental y las series animadas para adultxs, producidas por plataformas televisivas de streaming, puntualmente trata la enfermedad mental en la serie BoJack Horseman de Netflix. En la aproximación metodológica, realizada desde los estudios culturales, la autoetnografía, la investigación visual y los estudios de serialidad se mezclaron para dar cuenta de la coexistencia, que podría decirse necesaria, de la enfermedad mental como experiencia vivida —en este caso por una mujer y su familia—, con la de la enfermedad mental como experiencia animada —de la ficción, protagonizada por un caballo—, coexistencia en la que la presencia de las mujeres resulta, según mi opinión, ser parte clave para explicar lo que lxs críticxs, especialistas y seguidores consideran uno de los logros de la serie: tratar la enfermedad mental eludiendo los estigmas comunes, y hacerlo en un entorno mediático transmedial y transnacional.
La inclusión de la enfermedad mental en las producciones televisivas de Netflix, HBO y Amazon incrementó en los últimos diez años, a la par que la enfermedad mental como experiencia institucionalizada y medicalizada en empresas y universidades, más allá del contexto familiar. BoJack Horseman es una de las producciones que trata la enfermedad mental como una experiencia en la que se reconocen numerosas personas diagnosticadas con trastornos mentales en distinto grado. En la serie, la mayoría de los personajes diagnosticados son mujeres, de una misma línea genealógica que comparten la herencia genética y las preguntas por el sentido de la vida, la maternidad, el aborto, el éxito y la felicidad. Lo que sugiero es que las mujeres animadas de la serie tuvieron todo que ver con el equipo de mujeres directoras, creadoras, realizadoras, productoras e ilustradoras que dieron vida a BoJack Horseman y que reorientaron y modificaron sus propios diagnósticos sobre la enfermedad mental, para llevarlos a sus trabajos creativos en un proceso terapéutico y público que amplió la discusión sobre la enfermedad mental en la televisión y fuera de ella. Se trata desde los estudios culturales, de mujeres que tomaron agencia sobre sus propios diagnósticos.This research work identifies and suggests relationships between mental illness and adult animated TV series, produced by television streaming platforms, specifically I address mental illness in the original Netflix series BoJack Horseman. In the methodological approach, carried out from the field of cultural studies, autoethnography, visual research and seriality studies are mixed to account for the coexistence, which could be said to be necessary, of mental illness as a lived experience —in this case, of a woman and her family—, with that of mental illness as an animated experience — of fiction, starring a horse—, a coexistence in which the presence of women is, in my opinion, a key part in explaining what the critics, specialists and followers consider one of the achievements of the TV series: treating mental illness avoiding common stigmas, and doing it in a transmedia and transnational media environment.
The inclusion of mental illness in the television productions of Netflix, HBO and Amazon has increased in the last ten years, along with mental illness as an institutionalized and medical experience in companies and universities, beyond the family context. BoJack Horseman is one of the productions that treats mental illness as an experience in which numerous people who are diagnosed with mental disorders, to varying degrees, are recognized. In the series, most of the characters that are diagnosed are women, of the same genealogical line who share genetic inheritance and question the meaning of life, motherhood, abortion, success and happiness. What I suggest is that the animated women in the series had everything to do with the team of female directors, creators, filmmakers, producers and illustrators who were part of BoJack Horseman and who reoriented and modified their own diagnoses of mental illness, and took them to their creative works in a therapeutic and public process, which broadened the discussion about mental illness on the television screen and outside of it. From the field of cultural studies, this observation is about women who took agency over their own mental illness diagnoses.Línea de investigación: Códigos y prácticas expresivas y estéticasMaestrí
