Página de Pedro Autreto – Grupo de Estrutura Eletrônica e Dinâmica Atomística Interdisciplinar

Publicações de Pedro Autreto

2024
Quispe, Juan Gomez; Ipaves, Bruno; Galvao, Douglas Soares; Autreto, Pedro A. S.
TPDH-Graphene as a New Anodic Material for Lithium Ion Battery: DFT-Based Investigations Journal Article
Em: ACS Omega, vol. 0, não 0, pp. null, 2024.
Resumo | Links | BibTeX
@article{doi:10.1021/acsomega.4c06252,
title = {TPDH-Graphene as a New Anodic Material for Lithium Ion Battery: DFT-Based Investigations},
author = {Juan Gomez Quispe and Bruno Ipaves and Douglas Soares Galvao and Pedro A. S. Autreto},
url = {https://doi.org/10.1021/acsomega.4c06252},
doi = {10.1021/acsomega.4c06252},
year = {2024},
date = {2024-09-03},
urldate = {2024-09-03},
journal = {ACS Omega},
volume = {0},
number = {0},
pages = {null},
abstract = {The potential of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed 2D carbon allotrope as an anodic material in lithium ion batteries (LIBs), was investigated through density functional theory calculations. The results indicate that Li-atom adsorption is moderate (around 0.70 eV), allowing for easy desorption. Moreover, energy barriers (0.08–0.20 eV), diffusion coefficient (>6 × 10–6 cm2/s), and open circuit voltage (0.29 V) calculations show rapid Li atom diffusion on the TPDH-gr surface, stable intercalation of lithium atoms, and good performance during the charge and discharge cycles of the LIB. These findings, combined with the intrinsic metallic nature of TPDH-gr, indicate that this new 2D carbon allotrope is a promising candidate for use as an anodic LIB material.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
The potential of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed 2D carbon allotrope as an anodic material in lithium ion batteries (LIBs), was investigated through density functional theory calculations. The results indicate that Li-atom adsorption is moderate (around 0.70 eV), allowing for easy desorption. Moreover, energy barriers (0.08–0.20 eV), diffusion coefficient (>6 × 10–6 cm2/s), and open circuit voltage (0.29 V) calculations show rapid Li atom diffusion on the TPDH-gr surface, stable intercalation of lithium atoms, and good performance during the charge and discharge cycles of the LIB. These findings, combined with the intrinsic metallic nature of TPDH-gr, indicate that this new 2D carbon allotrope is a promising candidate for use as an anodic LIB material.
Fechar
https://doi.org/10.1021/acsomega.4c06252
doi:10.1021/acsomega.4c06252
Fechar
Chakraborty, Anyesha; Ipaves, Bruno; de Oliveira, Caique Campos; Negedu, Solomon Demiss; Sarkar, Suman; Lahiri, Basudev; Autreto, Pedro A. S.; Tiwary, Chandra Sekhar
Subpicomolar Dopamine Detection Using Two-Dimensional Cobalt Telluride Journal Article
Em: ACS Applied Engineering Materials, vol. 0, não 0, pp. null, 2024.
Resumo | Links | BibTeX
@article{doi:10.1021/acsaenm.4c00321,
title = {Subpicomolar Dopamine Detection Using Two-Dimensional Cobalt Telluride},
author = {Anyesha Chakraborty and Bruno Ipaves and Caique Campos de Oliveira and Solomon Demiss Negedu and Suman Sarkar and Basudev Lahiri and Pedro A. S. Autreto and Chandra Sekhar Tiwary},
url = {https://doi.org/10.1021/acsaenm.4c00321},
doi = {10.1021/acsaenm.4c00321},
year = {2024},
date = {2024-07-11},
journal = {ACS Applied Engineering Materials},
volume = {0},
number = {0},
pages = {null},
abstract = {To address the challenges associated with ultrasensitive dopamine sensing for regular health monitoring, here we developed a flexible sensor using two-dimensional cobalt telluride (2D CoTe2). The 2D-CoTe2-coated glassy carbon electrode sensor shows a limit of detection (LoD) of 0.21 pM measured by differential pulse voltammetry (DPV) in 0.1 M phosphate buffer solution (PBS). The assessment of selectivity, repeatability, and reproducibility has been conducted, to enquire about the efficiency of the sensor. The durability of the sensor has been verified for a duration of one month, demonstrating a minimal loss of 16% after a period of one month. The interaction of the 2D CoTe2 and dopamine has been investigated thoroughly by chemical fingerprints using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, and Raman imaging, and the adsorption of dopamine on 2D CoTe2 has been confirmed by the theoretical calculations calculating the binding energy, differential charge densities, and projected density of states (pDOS). Additionally, a flexible paper-based sensor using 2D CoTe2 has been successfully fabricated and employed for real-time dopamine detection from artificial sweat, which achieved a LoD of 0.22 pM.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
To address the challenges associated with ultrasensitive dopamine sensing for regular health monitoring, here we developed a flexible sensor using two-dimensional cobalt telluride (2D CoTe2). The 2D-CoTe2-coated glassy carbon electrode sensor shows a limit of detection (LoD) of 0.21 pM measured by differential pulse voltammetry (DPV) in 0.1 M phosphate buffer solution (PBS). The assessment of selectivity, repeatability, and reproducibility has been conducted, to enquire about the efficiency of the sensor. The durability of the sensor has been verified for a duration of one month, demonstrating a minimal loss of 16% after a period of one month. The interaction of the 2D CoTe2 and dopamine has been investigated thoroughly by chemical fingerprints using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, and Raman imaging, and the adsorption of dopamine on 2D CoTe2 has been confirmed by the theoretical calculations calculating the binding energy, differential charge densities, and projected density of states (pDOS). Additionally, a flexible paper-based sensor using 2D CoTe2 has been successfully fabricated and employed for real-time dopamine detection from artificial sweat, which achieved a LoD of 0.22 pM.
Fechar
https://doi.org/10.1021/acsaenm.4c00321
doi:10.1021/acsaenm.4c00321
Fechar
Quispe, Juan Gomez; Ipaves, Bruno; Galvao, Douglas Soares; Autreto, Pedro A. S.
TPDH-Graphene as a New Anodic Material for Lithium Ion Battery: DFT-Based Investigations Miscellaneous
2024.
Resumo | Links | BibTeX
@misc{quispe2024tpdhgraphenenewanodicmaterial,
title = {TPDH-Graphene as a New Anodic Material for Lithium Ion Battery: DFT-Based Investigations},
author = {Juan Gomez Quispe and Bruno Ipaves and Douglas Soares Galvao and Pedro A. S. Autreto},
url = {https://arxiv.org/abs/2407.04788},
doi = { https://doi.org/10.48550/arXiv.2407.04788},
year = {2024},
date = {2024-07-05},
urldate = {2024-01-01},
abstract = {The potential of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed 2D carbon allotrope as an anodic material in lithium ion batteries (LIB), was investigated through density functional theory (DFT) calculations. The results indicate that Li-atom adsorption is moderate (around 0.70 eV), allowing for easy desorption. Moreover, energy barrier, diffusion coefficient, and open circuit voltage (OCV) calculations show rapid Li atom diffusion on the TPDH-gr surface, stable intercalation of lithium atoms, and good performance during the charge and discharge cycles of the LIB. These findings, combined with the intrinsic metallic nature of TPDH-gr, indicate that this new 2D carbon allotrope is a promising candidate for use as an anodic LIB material. },
keywords = {},
pubstate = {published},
tppubtype = {misc}
}

Fechar
The potential of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed 2D carbon allotrope as an anodic material in lithium ion batteries (LIB), was investigated through density functional theory (DFT) calculations. The results indicate that Li-atom adsorption is moderate (around 0.70 eV), allowing for easy desorption. Moreover, energy barrier, diffusion coefficient, and open circuit voltage (OCV) calculations show rapid Li atom diffusion on the TPDH-gr surface, stable intercalation of lithium atoms, and good performance during the charge and discharge cycles of the LIB. These findings, combined with the intrinsic metallic nature of TPDH-gr, indicate that this new 2D carbon allotrope is a promising candidate for use as an anodic LIB material.
Fechar
https://arxiv.org/abs/2407.04788
doi: https://doi.org/10.48550/arXiv.2407.04788
Fechar
Cala, Paula; Dariani, Guilherme; Veiga, Eduardo; Macedo, Pedro; Paula, Amauri; de Almeida, James M.
Predictive Modeling of Surface Tension in Chemical Compounds: Uncovering Crucial Features with Machine Learning Journal Article
Em: J. Braz. Chem. Soc., 2024, ISSN: 1678-4790.
Resumo | Links | BibTeX
@article{Cala2024,
title = {Predictive Modeling of Surface Tension in Chemical Compounds: Uncovering Crucial Features with Machine Learning},
author = {Paula Cala and Guilherme Dariani and Eduardo Veiga and Pedro Macedo and Amauri Paula and James M. de Almeida},
doi = {10.21577/0103-5053.20240110},
issn = {1678-4790},
year = {2024},
date = {2024-07-01},
urldate = {2024-00-00},
journal = {J. Braz. Chem. Soc.},
publisher = {Sociedade Brasileira de Quimica (SBQ)},
abstract = {Surface tension (SFT) can shape the behavior of liquids in industrial chemical processes, influencing variables such as flow rate and separation efficiency. This property is commonly measured with experimental approaches such as Du Noüy ring and Wilhelmy plate methods. Here, we present machine learning (ML) methodologies that can predict the SFT of hydrocarbons. A comparative analysis encompassing k-nearest neighbors, random forest, and XGBoost (extreme gradient boosting) methods was done. Results from our study reveal that XGBoost is the most accurate in predicting hydrocarbon SFT, with a mean squared error (MSE) of 4.65 mN2 m-2 and a coefficient of determination (R2 ) score of 0.89. The feature importance was evaluated with the permutation feature importance method and Shapley analysis. Enthalpy of vaporization, density, molecular weight and hydrogen content are key factors in accurately predicting SFT. The successful integration of these methodologies holds the potential to impact efficiency in different industry processes.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Surface tension (SFT) can shape the behavior of liquids in industrial chemical processes, influencing variables such as flow rate and separation efficiency. This property is commonly measured with experimental approaches such as Du Noüy ring and Wilhelmy plate methods. Here, we present machine learning (ML) methodologies that can predict the SFT of hydrocarbons. A comparative analysis encompassing k-nearest neighbors, random forest, and XGBoost (extreme gradient boosting) methods was done. Results from our study reveal that XGBoost is the most accurate in predicting hydrocarbon SFT, with a mean squared error (MSE) of 4.65 mN2 m-2 and a coefficient of determination (R2 ) score of 0.89. The feature importance was evaluated with the permutation feature importance method and Shapley analysis. Enthalpy of vaporization, density, molecular weight and hydrogen content are key factors in accurately predicting SFT. The successful integration of these methodologies holds the potential to impact efficiency in different industry processes.
Fechar
doi:10.21577/0103-5053.20240110
Fechar
Quispe, Juan Gomez; Galvao, Douglas Soares; Autreto, Pedro A. S.
Exploring the Electronic and Mechanical Properties of TPDH-Nanotube: Insights from Ab initio and Classical Molecular Dynamics Simulations Working paper
2024.
Resumo | Links | BibTeX
@workingpaper{quispe2024exploringelectronicmechanicalproperties,
title = {Exploring the Electronic and Mechanical Properties of TPDH-Nanotube: Insights from Ab initio and Classical Molecular Dynamics Simulations},
author = {Juan Gomez Quispe and Douglas Soares Galvao and Pedro A. S. Autreto},
url = {https://arxiv.org/abs/2406.19536},
doi = {https://doi.org/10.48550/arXiv.2406.19536},
year = {2024},
date = {2024-06-27},
urldate = {2024-01-01},
abstract = {Tetra-Penta-Deca-Hexa-graphene (TPDH) is a new 2D carbon allotrope with attractive electronic and mechanical properties. It is composed of tetragonal, pentagonal, and hexagonal carbon rings. When TPDH-graphene is sliced into quasi-one-dimensional (1D) structures like nanoribbons, it exhibits a range of behaviors, from semi-metallic to semiconducting. An alternative approach to achieving these desirable electronic (electronic confinement and/or non-zero electronic band gap) properties is the creation of nanotubes (TPDH-NT). In the present work, we carried out a comprehensive study of TPDH-NTs combining Density Functional Theory (DFT) and Classical Reactive Molecular Dynamics (MD). Our results show structural stability and a chiral dependence on mechanical properties. Similarly to standard carbon nanotubes, TPDH-NT can be metallic or semiconductor. MD results show Young's modulus values exceeding 700 GPa, except for nanotubes with very small radii. However, certain chiral TPDH-NTs (n,m) display values both below and above 700 GPa, particularly for those with small radii. The analyses of the angle and C-C bond length distributions underscore the significance of the tetragonal and pentagonal rings in determining the mechanical response of TPDH-NTs (n,0) and (0,n), respectively. },
keywords = {},
pubstate = {published},
tppubtype = {workingpaper}
}

Fechar
Tetra-Penta-Deca-Hexa-graphene (TPDH) is a new 2D carbon allotrope with attractive electronic and mechanical properties. It is composed of tetragonal, pentagonal, and hexagonal carbon rings. When TPDH-graphene is sliced into quasi-one-dimensional (1D) structures like nanoribbons, it exhibits a range of behaviors, from semi-metallic to semiconducting. An alternative approach to achieving these desirable electronic (electronic confinement and/or non-zero electronic band gap) properties is the creation of nanotubes (TPDH-NT). In the present work, we carried out a comprehensive study of TPDH-NTs combining Density Functional Theory (DFT) and Classical Reactive Molecular Dynamics (MD). Our results show structural stability and a chiral dependence on mechanical properties. Similarly to standard carbon nanotubes, TPDH-NT can be metallic or semiconductor. MD results show Young's modulus values exceeding 700 GPa, except for nanotubes with very small radii. However, certain chiral TPDH-NTs (n,m) display values both below and above 700 GPa, particularly for those with small radii. The analyses of the angle and C-C bond length distributions underscore the significance of the tetragonal and pentagonal rings in determining the mechanical response of TPDH-NTs (n,0) and (0,n), respectively.
Fechar
https://arxiv.org/abs/2406.19536
doi:https://doi.org/10.48550/arXiv.2406.19536
Fechar
de Oliveira, Caique Campos; Galvão, Douglas S.; Autreto, Pedro A. S.
Selective Hydrogenation Promotes the Anisotropic Thermoelectric Properties of TPDH-Graphene Journal Article
Em: The Journal of Physical Chemistry C, vol. 128, não 15, pp. 6206-6212, 2024.
Resumo | Links | BibTeX
@article{doi:10.1021/acs.jpcc.4c00175,
title = {Selective Hydrogenation Promotes the Anisotropic Thermoelectric Properties of TPDH-Graphene},
author = {Caique Campos de Oliveira and Douglas S. Galvão and Pedro A. S. Autreto},
url = {https://doi.org/10.1021/acs.jpcc.4c00175},
doi = {10.1021/acs.jpcc.4c00175},
year = {2024},
date = {2024-03-28},
urldate = {2024-01-01},
journal = {The Journal of Physical Chemistry C},
volume = {128},
number = {15},
pages = {6206-6212},
abstract = {We have combined density functional theory calculations with the Boltzmann semiclassical transport theory to investigate the effect of selective hydrogenation on the thermoelectric properties of tetra-penta-decahexagonal graphene (TPDH-gr), a recently proposed new two-dimensional carbon allotrope. Our results show that the Seebeck coefficient is enhanced after hydrogenation. The conductivity along the x direction is increased almost eight times while being almost suppressed along the y direction. This behavior can be understood in terms of the electronic structure changes due to the appearance of a Dirac-like cone after selective hydrogenation. Consistent with the literature, the electronic contribution to the thermal conductivity displays the same qualitative behavior as the conductivity, as expected from the Wiedemann–Franz law. The increase in thermal conductivity with temperature limits the material’s power factor. The significant increases in the Seebeck coefficient and conductivity also contribute to the thermal conductivity increase. These results show that hydrogenation is an effective method to improve the TPDH-gr thermoelectric properties, and this carbon allotrope can be an effective material for thermoelectric applications.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
We have combined density functional theory calculations with the Boltzmann semiclassical transport theory to investigate the effect of selective hydrogenation on the thermoelectric properties of tetra-penta-decahexagonal graphene (TPDH-gr), a recently proposed new two-dimensional carbon allotrope. Our results show that the Seebeck coefficient is enhanced after hydrogenation. The conductivity along the x direction is increased almost eight times while being almost suppressed along the y direction. This behavior can be understood in terms of the electronic structure changes due to the appearance of a Dirac-like cone after selective hydrogenation. Consistent with the literature, the electronic contribution to the thermal conductivity displays the same qualitative behavior as the conductivity, as expected from the Wiedemann–Franz law. The increase in thermal conductivity with temperature limits the material’s power factor. The significant increases in the Seebeck coefficient and conductivity also contribute to the thermal conductivity increase. These results show that hydrogenation is an effective method to improve the TPDH-gr thermoelectric properties, and this carbon allotrope can be an effective material for thermoelectric applications.
Fechar
https://doi.org/10.1021/acs.jpcc.4c00175
doi:10.1021/acs.jpcc.4c00175
Fechar
Khatun, Salma; Alanwoko, Onyedikachi; Pathirage, Vimukthi; de Oliveira, Caique Campos; Tromer, Raphael M.; Autreto, Pedro A. S.; Galvao, Douglas S.; Batzill, Matthias
Solid State Reaction Epitaxy, A New Approach for Synthesizing Van der Waals heterolayers: The Case of Mn and Cr on Bi₂Se₃ Journal Article
Em: Adv Funct Materials, vol. 34, não 28, 2024, ISSN: 1616-3028.
Resumo | Links | BibTeX
@article{Khatun2024,
title = {Solid State Reaction Epitaxy, A New Approach for Synthesizing Van der Waals heterolayers: The Case of Mn and Cr on Bi_{2}Se_{3}},
author = {Salma Khatun and Onyedikachi Alanwoko and Vimukthi Pathirage and Caique Campos de Oliveira and Raphael M. Tromer and Pedro A. S. Autreto and Douglas S. Galvao and Matthias Batzill},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202315112},
doi = {10.1002/adfm.202315112},
issn = {1616-3028},
year = {2024},
date = {2024-03-12},
urldate = {2024-07-00},
journal = {Adv Funct Materials},
volume = {34},
number = {28},
publisher = {Wiley},
abstract = {AbstractVan der Waals (vdW) heterostructures that pair materials with diverse properties enable various quantum phenomena. However, the direct growth of vdW heterostructures is challenging. Modification of the surface layer of quantum materials to introduce new properties is an alternative process akin to solid state reaction. Here, vapor deposited transition metals (TMs), Cr and Mn, are reacted with Bi2Se3 with the goal to transform the surface layer to XBi2Se4 (X = Cr, Mn). Experiments and ab initio MD simulations demonstrate that the TMs have a high selenium affinity driving Se diffusion toward the TM. For monolayer Cr, the surface Bi2Se3 is reduced to Bi2‐layer and a stable (pseudo) 2D Cr1+δSe2 layer is formed. In contrast, monolayer Mn can transform upon mild annealing into MnBi2Se4. This phase only forms for a precise amount of initial Mn deposition. Sub‐monolayer amounts dissolve into the bulk, and multilayers form stable MnSe adlayers. This study highlights the delicate energy balance between adlayers and desired surface modified layers that governs the interface reactions and that the formation of stable adlayers can prevent the reaction with the substrate. The success of obtaining MnBi2Se4 points toward an approach for the engineering of other multicomponent vdW materials by surface reactions.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
AbstractVan der Waals (vdW) heterostructures that pair materials with diverse properties enable various quantum phenomena. However, the direct growth of vdW heterostructures is challenging. Modification of the surface layer of quantum materials to introduce new properties is an alternative process akin to solid state reaction. Here, vapor deposited transition metals (TMs), Cr and Mn, are reacted with Bi2Se3 with the goal to transform the surface layer to XBi2Se4 (X = Cr, Mn). Experiments and ab initio MD simulations demonstrate that the TMs have a high selenium affinity driving Se diffusion toward the TM. For monolayer Cr, the surface Bi2Se3 is reduced to Bi2‐layer and a stable (pseudo) 2D Cr1+δSe2 layer is formed. In contrast, monolayer Mn can transform upon mild annealing into MnBi2Se4. This phase only forms for a precise amount of initial Mn deposition. Sub‐monolayer amounts dissolve into the bulk, and multilayers form stable MnSe adlayers. This study highlights the delicate energy balance between adlayers and desired surface modified layers that governs the interface reactions and that the formation of stable adlayers can prevent the reaction with the substrate. The success of obtaining MnBi2Se4 points toward an approach for the engineering of other multicomponent vdW materials by surface reactions.
Fechar
https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202315112
doi:10.1002/adfm.202315112
Fechar
Bandeira, Lucas; Ferreira, Henrique; de Almeida, James M.; de Paula, Amauri Jardim; Dalpian, Gustavo Martini
CO2 Reduction beyond Copper-Based Catalysts: A Natural Language Processing Review from the Scientific Literature Journal Article
Em: ACS Sustainable Chemistry & Engineering, vol. 12, não 11, pp. 4411-4422, 2024.
Resumo | Links | BibTeX
@article{doi:10.1021/acssuschemeng.3c06920,
title = {CO2 Reduction beyond Copper-Based Catalysts: A Natural Language Processing Review from the Scientific Literature},
author = {Lucas Bandeira and Henrique Ferreira and James M. de Almeida and Amauri Jardim de Paula and Gustavo Martini Dalpian},
url = {https://doi.org/10.1021/acssuschemeng.3c06920},
doi = {10.1021/acssuschemeng.3c06920},
year = {2024},
date = {2024-03-06},
urldate = {2024-01-01},
journal = {ACS Sustainable Chemistry & Engineering},
volume = {12},
number = {11},
pages = {4411-4422},
abstract = {Carbon dioxide (CO2) is a prominent greenhouse gas that contributes significantly to global warming. To combat this issue, one strategy is the conversion of CO2 into alcohols and hydrocarbons, which can be used as fuels and chemical feedstocks. Consequently, a substantial volume of scientific literature has been dedicated to investigating different materials and reaction conditions to facilitate the CO2 reduction reaction (CO2RR) into these so-called high-value products. However, the vastness of this literature makes it challenging to stay updated on recent discoveries and review the most promising materials and conditions that have been explored. To address this issue, we applied natural language processing tools to extract valuable data from 7292 published articles in the scientific literature. Our analysis revealed the emergence of new materials such as cesium–lead–bromide perovskites and bismuth oxyhalides that have been recently used in the CO2RR and identified Bi-based catalysts as the most selective for HCOO– production. Furthermore, we gleaned insights into the composition of other elements and materials commonly employed in the CO2RR, their relationship to product distribution, and the prevalent electrolytes used in the CO2 electrochemical reduction. Our findings can serve as a foundation for future investigations in the realm of catalysts for CO2RRs, offering insights into the most promising materials and conditions to pursue further research.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Carbon dioxide (CO2) is a prominent greenhouse gas that contributes significantly to global warming. To combat this issue, one strategy is the conversion of CO2 into alcohols and hydrocarbons, which can be used as fuels and chemical feedstocks. Consequently, a substantial volume of scientific literature has been dedicated to investigating different materials and reaction conditions to facilitate the CO2 reduction reaction (CO2RR) into these so-called high-value products. However, the vastness of this literature makes it challenging to stay updated on recent discoveries and review the most promising materials and conditions that have been explored. To address this issue, we applied natural language processing tools to extract valuable data from 7292 published articles in the scientific literature. Our analysis revealed the emergence of new materials such as cesium–lead–bromide perovskites and bismuth oxyhalides that have been recently used in the CO2RR and identified Bi-based catalysts as the most selective for HCOO– production. Furthermore, we gleaned insights into the composition of other elements and materials commonly employed in the CO2RR, their relationship to product distribution, and the prevalent electrolytes used in the CO2 electrochemical reduction. Our findings can serve as a foundation for future investigations in the realm of catalysts for CO2RRs, offering insights into the most promising materials and conditions to pursue further research.
Fechar
https://doi.org/10.1021/acssuschemeng.3c06920
doi:10.1021/acssuschemeng.3c06920
Fechar
Moura, João Paulo C.; Lucchetti, Lanna E. B.; Fernandes, Caio M.; Trench, Aline B.; Lange, Camila N.; Batista, Bruno L.; de Almeida, James M.; Santos, Mauro C.
Experimental and theoretical studies of WO3/Vulcan XC-72 electrocatalyst enhanced H2O2 yield ORR performed in acid and alkaline medium Journal Article
Em: Journal of Environmental Chemical Engineering, vol. 12, não 4, pp. 113182, 2024, ISSN: 2213-3437.
Resumo | Links | BibTeX
@article{MOURA2024113182,
title = {Experimental and theoretical studies of WO3/Vulcan XC-72 electrocatalyst enhanced H2O2 yield ORR performed in acid and alkaline medium},
author = {João Paulo C. Moura and Lanna E. B. Lucchetti and Caio M. Fernandes and Aline B. Trench and Camila N. Lange and Bruno L. Batista and James M. de Almeida and Mauro C. Santos},
url = {https://www.sciencedirect.com/science/article/pii/S2213343724013125},
doi = {https://doi.org/10.1016/j.jece.2024.113182},
issn = {2213-3437},
year = {2024},
date = {2024-03-06},
urldate = {2024-01-01},
journal = {Journal of Environmental Chemical Engineering},
volume = {12},
number = {4},
pages = {113182},
abstract = {The oxygen reduction reaction (ORR) plays a pivotal role in clean energy generation and sustainable chemical production, particularly in the synthesis of hydrogen peroxide (H2O2). In this study, WO3/Vulcan-XC72 electrocatalysts have been synthesized and characterized for ORR applications. We assessed the ratio of WO3 to Vulcan-XC72 and investigated the impact of electrolytes pH (covering acidic and alkaline media) on the ORR process. The results revealed that WO3 with a monoclinic crystalline phase and nanoflower-like morphology was successfully synthesized, and confirmed an improvement in surface properties, with an increase in hydrophilicity and superficial oxygenated species. Electrochemical studies showed that WO3/C was the most selective for H2O2 electrogeneration, compared to pure Vulcan-XC72, in both acidic and alkaline media. These results indicate that the ORR on the WO3/C electrocatalyst surface has a pH-dependent mechanism. Using WO3/C GDEs, an accumulation of 862 mg L-1 of H2O2 was achieved after 120 min of electrolysis at 100 mA cm-2. The higher selectivity of WO3/C could be related to the presence of more oxygen functional acid species on the catalyst surface and increased hydrophilicity compared to pure Vulcan, as well as a synergistic effect of the WO3 nanoflowers in ORR, confirmed by theoretical calculations. The results reveal that WO3/Vulcan is a promising catalyst for H2O2 electrogeneration via the ORR.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
The oxygen reduction reaction (ORR) plays a pivotal role in clean energy generation and sustainable chemical production, particularly in the synthesis of hydrogen peroxide (H2O2). In this study, WO3/Vulcan-XC72 electrocatalysts have been synthesized and characterized for ORR applications. We assessed the ratio of WO3 to Vulcan-XC72 and investigated the impact of electrolytes pH (covering acidic and alkaline media) on the ORR process. The results revealed that WO3 with a monoclinic crystalline phase and nanoflower-like morphology was successfully synthesized, and confirmed an improvement in surface properties, with an increase in hydrophilicity and superficial oxygenated species. Electrochemical studies showed that WO3/C was the most selective for H2O2 electrogeneration, compared to pure Vulcan-XC72, in both acidic and alkaline media. These results indicate that the ORR on the WO3/C electrocatalyst surface has a pH-dependent mechanism. Using WO3/C GDEs, an accumulation of 862 mg L-1 of H2O2 was achieved after 120 min of electrolysis at 100 mA cm-2. The higher selectivity of WO3/C could be related to the presence of more oxygen functional acid species on the catalyst surface and increased hydrophilicity compared to pure Vulcan, as well as a synergistic effect of the WO3 nanoflowers in ORR, confirmed by theoretical calculations. The results reveal that WO3/Vulcan is a promising catalyst for H2O2 electrogeneration via the ORR.
Fechar
https://www.sciencedirect.com/science/article/pii/S2213343724013125
doi:https://doi.org/10.1016/j.jece.2024.113182
Fechar
Lucchetti, Lanna E. B.; Autreto, Pedro A. S.; Santos, Mauro C.; de Almeida, James M.
Cerium doped graphene-based materials towards oxygen reduction reaction catalysis Journal Article
Em: Materials Today Communications, vol. 38, pp. 108461, 2024, ISSN: 2352-4928.
Resumo | Links | BibTeX
@article{LUCCHETTI2024108461,
title = {Cerium doped graphene-based materials towards oxygen reduction reaction catalysis},
author = {Lanna E. B. Lucchetti and Pedro A. S. Autreto and Mauro C. Santos and James M. de Almeida},
url = {https://www.sciencedirect.com/science/article/pii/S2352492824004410},
doi = {https://doi.org/10.1016/j.mtcomm.2024.108461},
issn = {2352-4928},
year = {2024},
date = {2024-02-23},
urldate = {2024-01-01},
journal = {Materials Today Communications},
volume = {38},
pages = {108461},
abstract = {With the global transition towards cleaner energy and sustainable processes, the demand for efficient catalysts, especially for the oxygen reduction reaction, has gained attention from the scientific community. This research work investigates cerium-doped graphene-based materials as catalysts for this process with density functional theory calculations. The electrochemical performance of Ce-doped graphene was assessed within the computation hydrogen electrode framework. Our findings reveal that Ce doping, especially when synergized with an oxygen atom, shows improved catalytic activity and selectivity. For instance, Ce doping in combination with an oxygen atom, located near a border, can be selective for the 2-electron pathway. Overall, the combination of Ce doping with structural defects and oxygenated functions lowers the reaction free energies for the oxygen reduction compared to pure graphene, and consequently, might improve the catalytic activity. This research sheds light from a computational perspective on Ce-doped carbon materials as a sustainable alternative to traditional costly metal-based catalysts, offering promising prospects for green energy technologies and electrochemical applications.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
With the global transition towards cleaner energy and sustainable processes, the demand for efficient catalysts, especially for the oxygen reduction reaction, has gained attention from the scientific community. This research work investigates cerium-doped graphene-based materials as catalysts for this process with density functional theory calculations. The electrochemical performance of Ce-doped graphene was assessed within the computation hydrogen electrode framework. Our findings reveal that Ce doping, especially when synergized with an oxygen atom, shows improved catalytic activity and selectivity. For instance, Ce doping in combination with an oxygen atom, located near a border, can be selective for the 2-electron pathway. Overall, the combination of Ce doping with structural defects and oxygenated functions lowers the reaction free energies for the oxygen reduction compared to pure graphene, and consequently, might improve the catalytic activity. This research sheds light from a computational perspective on Ce-doped carbon materials as a sustainable alternative to traditional costly metal-based catalysts, offering promising prospects for green energy technologies and electrochemical applications.
Fechar
https://www.sciencedirect.com/science/article/pii/S2352492824004410
doi:https://doi.org/10.1016/j.mtcomm.2024.108461
Fechar
Trench, Aline B.; Fernandes, Caio Machado; Moura, João Paulo C.; Lucchetti, Lanna E. B.; Lima, Thays S.; Antonin, Vanessa S.; de Almeida, James M.; Autreto, Pedro A. S.; Robles, Irma; Motheo, Artur J.; Lanza, Marcos R. V.; Santos, Mauro C.
Hydrogen peroxide electrogeneration from O2 electroreduction: A review focusing on carbon electrocatalysts and environmental applications Journal Article
Em: Chemosphere, pp. 141456, 2024, ISSN: 0045-6535.
Resumo | Links | BibTeX
@article{TRENCH2024141456,
title = {Hydrogen peroxide electrogeneration from O2 electroreduction: A review focusing on carbon electrocatalysts and environmental applications},
author = {Aline B. Trench and Caio Machado Fernandes and João Paulo C. Moura and Lanna E. B. Lucchetti and Thays S. Lima and Vanessa S. Antonin and James M. de Almeida and Pedro A. S. Autreto and Irma Robles and Artur J. Motheo and Marcos R. V. Lanza and Mauro C. Santos},
url = {https://www.sciencedirect.com/science/article/pii/S0045653524003497},
doi = {https://doi.org/10.1016/j.chemosphere.2024.141456},
issn = {0045-6535},
year = {2024},
date = {2024-02-15},
urldate = {2024-02-15},
journal = {Chemosphere},
pages = {141456},
abstract = {Hydrogen peroxide (H2O2) stands as one of the foremost utilized oxidizing agents in modern times. The established method for its production involves the intricate and costly anthraquinone process. However, a promising alternative pathway is the electrochemical hydrogen peroxide production, accomplished through the oxygen reduction reaction via a 2-electron pathway. This method not only simplifies the production process but also upholds environmental sustainability, especially when compared to the conventional anthraquinone method. In this review paper, recent works from the literature focusing on the 2-electron oxygen reduction reaction promoted by carbon electrocatalysts are summarized. The practical applications of these materials in the treatment of effluents contaminated with different pollutants (drugs, dyes, pesticides, and herbicides) are presented. Water treatment aiming to address these issues can be achieved through advanced oxidation electrochemical processes such as electro-Fenton, solar-electro-Fenton, and photo-electro-Fenton. These processes are discussed in detail in this work and the possible radicals that degrade the pollutants in each case are highlighted. The review broadens its scope to encompass contemporary computational simulations focused on the 2-electron oxygen reduction reaction, employing different models to describe carbon-based electrocatalysts. Finally, perspectives and future challenges in the area of carbon-based electrocatalysts for H2O2 electrogeneration are discussed. This review paper presents a forward-oriented viewpoint of present innovations and pragmatic implementations, delineating forthcoming challenges and prospects of this ever-evolving field.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Hydrogen peroxide (H2O2) stands as one of the foremost utilized oxidizing agents in modern times. The established method for its production involves the intricate and costly anthraquinone process. However, a promising alternative pathway is the electrochemical hydrogen peroxide production, accomplished through the oxygen reduction reaction via a 2-electron pathway. This method not only simplifies the production process but also upholds environmental sustainability, especially when compared to the conventional anthraquinone method. In this review paper, recent works from the literature focusing on the 2-electron oxygen reduction reaction promoted by carbon electrocatalysts are summarized. The practical applications of these materials in the treatment of effluents contaminated with different pollutants (drugs, dyes, pesticides, and herbicides) are presented. Water treatment aiming to address these issues can be achieved through advanced oxidation electrochemical processes such as electro-Fenton, solar-electro-Fenton, and photo-electro-Fenton. These processes are discussed in detail in this work and the possible radicals that degrade the pollutants in each case are highlighted. The review broadens its scope to encompass contemporary computational simulations focused on the 2-electron oxygen reduction reaction, employing different models to describe carbon-based electrocatalysts. Finally, perspectives and future challenges in the area of carbon-based electrocatalysts for H2O2 electrogeneration are discussed. This review paper presents a forward-oriented viewpoint of present innovations and pragmatic implementations, delineating forthcoming challenges and prospects of this ever-evolving field.
Fechar
https://www.sciencedirect.com/science/article/pii/S0045653524003497
doi:https://doi.org/10.1016/j.chemosphere.2024.141456
Fechar
de Oliveira, Caique Campos; Galvao, Douglas Soares; Autreto, Pedro A. S.
Selective Hydrogenation Promotes Anisotropic Thermoelectric Properties of TPDH-Graphene Working paper
2024.
Resumo | Links | BibTeX
@workingpaper{deoliveira2024selective,
title = {Selective Hydrogenation Promotes Anisotropic Thermoelectric Properties of TPDH-Graphene},
author = {Caique Campos de Oliveira and Douglas Soares Galvao and Pedro A. S. Autreto},
url = {https://arxiv.org/abs/2402.09572},
doi = { https://doi.org/10.48550/arXiv.2402.09572},
year = {2024},
date = {2024-02-14},
urldate = {2024-02-14},
abstract = {We have combined DFT calculations with the Boltzmann semiclassical transport theory to investigate the effect of selective hydrogenation on the thermoelectric properties of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed new 2D carbon allotrope. Our results show that the Seebeck coefficient is enhanced after hydrogenation. The conductivity along the x direction is increased almost eight times while being almost suppressed along the y direction. This behavior can be understood in terms of the electronic structure changes due to the appearance of a Dirac-like cone after the selective hydrogenation. Consistent with the literature, the electronic contribution to thermal conductivity displays the same qualitative behavior as the conductivity, as expected from the Wiedemann-Franz law. The increase in thermal conductivity with temperature limits the material's power factor. The significant increase in the Seebeck coefficient and conductivity increases also contribute to the thermal conductivity increase. These results show that hydrogenation is an effective method to improve the TPDH-gr thermoelectric properties, and this carbon allotrope can be an effective material for thermoelectric applications.},
keywords = {},
pubstate = {published},
tppubtype = {workingpaper}
}

Fechar
We have combined DFT calculations with the Boltzmann semiclassical transport theory to investigate the effect of selective hydrogenation on the thermoelectric properties of tetra-penta-deca-hexagonal graphene (TPDH-gr), a recently proposed new 2D carbon allotrope. Our results show that the Seebeck coefficient is enhanced after hydrogenation. The conductivity along the x direction is increased almost eight times while being almost suppressed along the y direction. This behavior can be understood in terms of the electronic structure changes due to the appearance of a Dirac-like cone after the selective hydrogenation. Consistent with the literature, the electronic contribution to thermal conductivity displays the same qualitative behavior as the conductivity, as expected from the Wiedemann-Franz law. The increase in thermal conductivity with temperature limits the material’s power factor. The significant increase in the Seebeck coefficient and conductivity increases also contribute to the thermal conductivity increase. These results show that hydrogenation is an effective method to improve the TPDH-gr thermoelectric properties, and this carbon allotrope can be an effective material for thermoelectric applications.
Fechar
https://arxiv.org/abs/2402.09572
doi: https://doi.org/10.48550/arXiv.2402.09572
Fechar
2023
Almeida, Tielle M.; de Almeida, James M.; Kudrna, Kathiane B.; Emanuelli, Tatiana; Leite, Daiani C.; Frizzo, Clarissa P.; Paz, Alisson V.; Schaffazick, Scheila R.; Silva, Cristiane
Photostable Ferulic Acid-Loaded Nanoemulsion for Anti-inflammatory Skin Application Journal Article
Em: ACS Applied Nano Materials, vol. 6, não 24, pp. 22807-22817, 2023.
Resumo | Links | BibTeX
@article{doi:10.1021/acsanm.3c03980,
title = {Photostable Ferulic Acid-Loaded Nanoemulsion for Anti-inflammatory Skin Application},
author = {Tielle M. Almeida and James M. de Almeida and Kathiane B. Kudrna and Tatiana Emanuelli and Daiani C. Leite and Clarissa P. Frizzo and Alisson V. Paz and Scheila R. Schaffazick and Cristiane Silva},
url = {https://doi.org/10.1021/acsanm.3c03980},
doi = {10.1021/acsanm.3c03980},
year = {2023},
date = {2023-12-13},
urldate = {2023-01-01},
journal = {ACS Applied Nano Materials},
volume = {6},
number = {24},
pages = {22807-22817},
abstract = {Ferulic acid (FA) is a highly promising phenolic compound known for its pharmacological activities, which include antioxidant, anti-inflammatory, and anticancer properties. However, limited bioavailability and low solubility hinder their therapeutic application. To overcome these challenges, nanocarriers can be designed by using computer simulation studies to enhance performance and stability. Classical molecular dynamics (CMD), widely employed to study interfaces, especially water–oil interfaces, plays a vital role in predicting molecular interactions and guiding the development of more efficient and effective drug delivery systems. Thus, this study aimed to develop FA nanoemulsions containing hazelnut oil (NE-FAHO) or medium-chain triglycerides (NE-FAMCT) with a previous study about the components that constitute the nanoemulsion and interfacial tension by CMD simulation. The FA-loaded nanoemulsions were prepared by the spontaneous emulsification method, and four different concentrations were used: 0.5 to 2.0 mg/mL. The nanoemulsions were characterized by measuring their droplet size, zeta potential, pH, FA content, encapsulation efficiency, and morphology. In addition, the stability and photostability of the FA nanoemulsions were evaluated. Analyzing the concentrations tested, NE-FAMCT at 1.5 mg/mL exhibited the best results in terms of characterization and stability, maintaining a content close to 95% for 60 days and providing photoprotection to FA. Furthermore, NE-FAMCT presented controlled release and significant antioxidant effect. Considering the significant FA anti-inflammatory and antioxidant potential, this study may contribute to the future development of topical pharmaceutical formulations aimed at treating skin-related diseases.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Ferulic acid (FA) is a highly promising phenolic compound known for its pharmacological activities, which include antioxidant, anti-inflammatory, and anticancer properties. However, limited bioavailability and low solubility hinder their therapeutic application. To overcome these challenges, nanocarriers can be designed by using computer simulation studies to enhance performance and stability. Classical molecular dynamics (CMD), widely employed to study interfaces, especially water–oil interfaces, plays a vital role in predicting molecular interactions and guiding the development of more efficient and effective drug delivery systems. Thus, this study aimed to develop FA nanoemulsions containing hazelnut oil (NE-FAHO) or medium-chain triglycerides (NE-FAMCT) with a previous study about the components that constitute the nanoemulsion and interfacial tension by CMD simulation. The FA-loaded nanoemulsions were prepared by the spontaneous emulsification method, and four different concentrations were used: 0.5 to 2.0 mg/mL. The nanoemulsions were characterized by measuring their droplet size, zeta potential, pH, FA content, encapsulation efficiency, and morphology. In addition, the stability and photostability of the FA nanoemulsions were evaluated. Analyzing the concentrations tested, NE-FAMCT at 1.5 mg/mL exhibited the best results in terms of characterization and stability, maintaining a content close to 95% for 60 days and providing photoprotection to FA. Furthermore, NE-FAMCT presented controlled release and significant antioxidant effect. Considering the significant FA anti-inflammatory and antioxidant potential, this study may contribute to the future development of topical pharmaceutical formulations aimed at treating skin-related diseases.
Fechar
https://doi.org/10.1021/acsanm.3c03980
doi:10.1021/acsanm.3c03980
Fechar
de Almeida, James M.; Ferreira, Conny Cerai; Bandeira, Lucas; Cunha, Renato D.; Coutinho-Neto, Mauricio Domingues; Homem-De-Mello, Paula; Orestes, Ednilsom; Nascimento, Regina Sandra Veiga
Synergistic Interaction of Hyperbranched Polyglycerols and Cetyltrimethylammonium Bromide for Oil/Water Interfacial Tension Reduction: A Molecular Dynamics Study Journal Article
Em: The Journal of Physical Chemistry B, vol. 127, não 43, pp. 9356-9365, 2023, (PMID: 37871185).
Resumo | Links | BibTeX
@article{doi:10.1021/acs.jpcb.3c01707,
title = {Synergistic Interaction of Hyperbranched Polyglycerols and Cetyltrimethylammonium Bromide for Oil/Water Interfacial Tension Reduction: A Molecular Dynamics Study},
author = {James M. de Almeida and Conny Cerai Ferreira and Lucas Bandeira and Renato D. Cunha and Mauricio Domingues Coutinho-Neto and Paula Homem-De-Mello and Ednilsom Orestes and Regina Sandra Veiga Nascimento},
url = {https://doi.org/10.1021/acs.jpcb.3c01707},
doi = {10.1021/acs.jpcb.3c01707},
year = {2023},
date = {2023-10-23},
urldate = {2023-01-01},
journal = {The Journal of Physical Chemistry B},
volume = {127},
number = {43},
pages = {9356-9365},
abstract = {Applying surfactants to reduce the interfacial tension (IFT) on water/oil interfaces is a proven technique. The search for new surfactants and delivery strategies is an ongoing research area with applications in many fields such as drug delivery through nanoemulsions and enhanced oil recovery. Experimentally, the combination of hyperbranched polyglycerol (HPG) with cetyltrimethylammonium bromide (CTAB) substantially reduced the observed IFT of oil/water interface, 0.9 mN/m, while HPG alone was 5.80 mN/m and CTAB alone IFT was 8.08 mN/m. Previous simulations in an aqueous solution showed that HPG is a surfactant carrier. Complementarily, in this work, we performed classical molecular dynamics simulations on combinations of CTAB and HPG with one aliphatic chain to investigate further the interaction of this pair in oil interfaces and propose the mechanism of IFT decrease. Basically, from our results, one can observe that the IFT reduction comes from a combination of effects that have not been observed for other dual systems: (i) Due to the CTAB-HPG strong interaction, a weakening of their specific and isolated interactions with the water and oil phases occurs. (ii) Aggregates enlarge the interfacial area, turning it into a less ordered interface. (iii) The spread of individual molecules charge profiles leads to the much lower interfacial tension observed with the CTAB+HPG systems.},
note = {PMID: 37871185},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Applying surfactants to reduce the interfacial tension (IFT) on water/oil interfaces is a proven technique. The search for new surfactants and delivery strategies is an ongoing research area with applications in many fields such as drug delivery through nanoemulsions and enhanced oil recovery. Experimentally, the combination of hyperbranched polyglycerol (HPG) with cetyltrimethylammonium bromide (CTAB) substantially reduced the observed IFT of oil/water interface, 0.9 mN/m, while HPG alone was 5.80 mN/m and CTAB alone IFT was 8.08 mN/m. Previous simulations in an aqueous solution showed that HPG is a surfactant carrier. Complementarily, in this work, we performed classical molecular dynamics simulations on combinations of CTAB and HPG with one aliphatic chain to investigate further the interaction of this pair in oil interfaces and propose the mechanism of IFT decrease. Basically, from our results, one can observe that the IFT reduction comes from a combination of effects that have not been observed for other dual systems: (i) Due to the CTAB-HPG strong interaction, a weakening of their specific and isolated interactions with the water and oil phases occurs. (ii) Aggregates enlarge the interfacial area, turning it into a less ordered interface. (iii) The spread of individual molecules charge profiles leads to the much lower interfacial tension observed with the CTAB+HPG systems.
Fechar
https://doi.org/10.1021/acs.jpcb.3c01707
doi:10.1021/acs.jpcb.3c01707
Fechar
Mahapatra, Preeti Lata; de Oliveira, Caique Campos; Sreeram, P. R.; Sivaraman, Sivaraj Kanneth; Sarkar, Suman; Costin, Gelu; Lahiri, Basudev; Autreto, Pedro A. S.; Tiwary, Chandra Sekhar
Hydrogen Sulfide Gas Detection Using Two-Dimensional Rhodonite Silicate Journal Article
Em: Chemistry of Materials, 2023.
Resumo | Links | BibTeX
@article{doi:10.1021/acs.chemmater.3c01593,
title = {Hydrogen Sulfide Gas Detection Using Two-Dimensional Rhodonite Silicate},
author = {Preeti Lata Mahapatra and Caique Campos de Oliveira and P. R. Sreeram and Sivaraj Kanneth Sivaraman and Suman Sarkar and Gelu Costin and Basudev Lahiri and Pedro A. S. Autreto and Chandra Sekhar Tiwary},
url = {https://doi.org/10.1021/acs.chemmater.3c01593},
doi = {10.1021/acs.chemmater.3c01593},
year = {2023},
date = {2023-09-22},
urldate = {2023-09-22},
journal = {Chemistry of Materials},
abstract = {Hydrogen sulfide is a hazardous gas that is found in common industrial waste sources, including sewage and oil refineries; it is lethal at concentrations exceeding 100 ppm. Two-dimensional (2D) oxide materials with a high surface area and environmental stability can be utilized for ultralow concentration gas sensing (H2S gas). Here, we demonstrate the gas sensing properties of two-dimensional rhodonite silicate (R-silicate) extracted from natural mineral ore. 2D R-silicate shows high sensitivity of up to 0.2 ppm–1 and high selectivity toward H2S compared to CO2, ethanol, acetone, and ammonia. The sensors developed using 2D R-silicate are found to be stable after five months. The high surface area and composition consisting of Mn atoms play a significant role in the sensing behavior. Ab initio computing simulations explain the mechanism of the selectivity of H2S over CO2 using 2D R-silicate. The simulation also demonstrates the chemical interaction of H2S with the 2D surface of R-silicate, which is further supported by Raman spectroscopy. The findings of this study provide new opportunities for using environmentally stable natural silicate 2D materials as efficient replacements for conventional metal oxides for ultrasensitive sensors.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Hydrogen sulfide is a hazardous gas that is found in common industrial waste sources, including sewage and oil refineries; it is lethal at concentrations exceeding 100 ppm. Two-dimensional (2D) oxide materials with a high surface area and environmental stability can be utilized for ultralow concentration gas sensing (H2S gas). Here, we demonstrate the gas sensing properties of two-dimensional rhodonite silicate (R-silicate) extracted from natural mineral ore. 2D R-silicate shows high sensitivity of up to 0.2 ppm–1 and high selectivity toward H2S compared to CO2, ethanol, acetone, and ammonia. The sensors developed using 2D R-silicate are found to be stable after five months. The high surface area and composition consisting of Mn atoms play a significant role in the sensing behavior. Ab initio computing simulations explain the mechanism of the selectivity of H2S over CO2 using 2D R-silicate. The simulation also demonstrates the chemical interaction of H2S with the 2D surface of R-silicate, which is further supported by Raman spectroscopy. The findings of this study provide new opportunities for using environmentally stable natural silicate 2D materials as efficient replacements for conventional metal oxides for ultrasensitive sensors.
Fechar
https://doi.org/10.1021/acs.chemmater.3c01593
doi:10.1021/acs.chemmater.3c01593
Fechar
Buzelli, Thiago; Ipaves, Bruno; Almeida, Wanda Pereira; Galvao, Douglas Soares; Autreto, Pedro A. S.
Machine Learning-based Analysis of Electronic Properties as Predictors of Anticholinesterase Activity in Chalcone Derivatives Working paper
2023.
Resumo | Links | BibTeX
@workingpaper{buzelli2023machine,
title = {Machine Learning-based Analysis of Electronic Properties as Predictors of Anticholinesterase Activity in Chalcone Derivatives},
author = {Thiago Buzelli and Bruno Ipaves and Wanda Pereira Almeida and Douglas Soares Galvao and Pedro A. S. Autreto},
url = {https://arxiv.org/abs/2309.07312},
doi = {10.48550/arXiv.2309.07312},
year = {2023},
date = {2023-09-13},
urldate = {2023-01-01},
abstract = {In this study, we investigated the correlation between the electronic properties of anticholinesterase compounds and their biological activity. While the methodology of such correlation is well-established and has been effectively utilized in previous studies, we employed a more sophisticated approach: machine learning. Initially, we focused on a set of 22 molecules sharing a common chalcone skeleton and categorized them into two groups based on their IC50 indices: active and inactive. Utilizing the open-source software Orca, we conducted calculations to determine the geometries and electronic structures of these molecules. Over a hundred parameters were collected from these calculations, serving as the foundation for the features used in machine learning. These parameters included the Mulliken and Lowdin electronic populations of each atom within the skeleton, molecular orbital energies, and Mayer's free valences. Through our analysis, we developed numerous models and identified several successful candidates for effectively distinguishing between the two groups. Notably, the most informative descriptor for this separation relied solely on electronic populations and orbital energies. By understanding which computationally calculated properties are most relevant to specific biological activities, we can significantly enhance the efficiency of drug development processes, saving both time and resources.},
keywords = {},
pubstate = {published},
tppubtype = {workingpaper}
}

Fechar
In this study, we investigated the correlation between the electronic properties of anticholinesterase compounds and their biological activity. While the methodology of such correlation is well-established and has been effectively utilized in previous studies, we employed a more sophisticated approach: machine learning. Initially, we focused on a set of 22 molecules sharing a common chalcone skeleton and categorized them into two groups based on their IC50 indices: active and inactive. Utilizing the open-source software Orca, we conducted calculations to determine the geometries and electronic structures of these molecules. Over a hundred parameters were collected from these calculations, serving as the foundation for the features used in machine learning. These parameters included the Mulliken and Lowdin electronic populations of each atom within the skeleton, molecular orbital energies, and Mayer’s free valences. Through our analysis, we developed numerous models and identified several successful candidates for effectively distinguishing between the two groups. Notably, the most informative descriptor for this separation relied solely on electronic populations and orbital energies. By understanding which computationally calculated properties are most relevant to specific biological activities, we can significantly enhance the efficiency of drug development processes, saving both time and resources.
Fechar
https://arxiv.org/abs/2309.07312
doi:10.48550/arXiv.2309.07312
Fechar
Sousa, J M De; Machado, L D; Woellner, C F; Medina, Matheus; Autreto, Pedro A. S.; Galvão, D S
Boron nitride nanotube peapods at ultrasonic velocity impacts: a fully atomistic molecular dynamics investigation Journal Article
Em: J. Phys.: Condens. Matter, vol. 35, não 33, 2023, ISSN: 1361-648X.
Resumo | Links | BibTeX
@article{DeSousa2023,
title = {Boron nitride nanotube peapods at ultrasonic velocity impacts: a fully atomistic molecular dynamics investigation},
author = {J M De Sousa and L D Machado and C F Woellner and Matheus Medina and Pedro A. S. Autreto and D S Galvão},
doi = {10.1088/1361-648x/acd50b},
issn = {1361-648X},
year = {2023},
date = {2023-08-23},
urldate = {2023-08-23},
journal = {J. Phys.: Condens. Matter},
volume = {35},
number = {33},
publisher = {IOP Publishing},
abstract = {Abstract
Boron nitride nanotube peapods (BNNT-peapod) are composed of linear chains of C60 molecules encapsulated inside BNNTs, they were first synthesized in 2003. In this work, we investigated the mechanical response and fracture dynamics of BNNT-peapods under ultrasonic velocity impacts (from 1 km s−1 up to 6 km s−1) against a solid target. We carried out fully atomistic reactive molecular dynamics simulations using a reactive force field. We have considered the case of horizontal and vertical shootings. Depending on the velocity values, we observed tube bending, tube fracture, and C60 ejection. Furthermore, the nanotube unzips for horizontal impacts at certain speeds, forming bi-layer nanoribbons ‘incrusted’ with C60 molecules. The methodology used here is applicable to other nanostructures. We hope it motivates other theoretical investigations on the behavior of nanostructures at ultrasonic velocity impacts and aid in interpreting future experimental results. It should be stressed that similar experiments and simulations were carried out on carbon nanotubes trying to obtain nanodiamonds. The present study expands these investigations to include BNNT.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Abstract
Boron nitride nanotube peapods (BNNT-peapod) are composed of linear chains of C60 molecules encapsulated inside BNNTs, they were first synthesized in 2003. In this work, we investigated the mechanical response and fracture dynamics of BNNT-peapods under ultrasonic velocity impacts (from 1 km s−1 up to 6 km s−1) against a solid target. We carried out fully atomistic reactive molecular dynamics simulations using a reactive force field. We have considered the case of horizontal and vertical shootings. Depending on the velocity values, we observed tube bending, tube fracture, and C60 ejection. Furthermore, the nanotube unzips for horizontal impacts at certain speeds, forming bi-layer nanoribbons ‘incrusted’ with C60 molecules. The methodology used here is applicable to other nanostructures. We hope it motivates other theoretical investigations on the behavior of nanostructures at ultrasonic velocity impacts and aid in interpreting future experimental results. It should be stressed that similar experiments and simulations were carried out on carbon nanotubes trying to obtain nanodiamonds. The present study expands these investigations to include BNNT.
Fechar
doi:10.1088/1361-648x/acd50b
Fechar
Antonin, Vanessa S.; Lucchetti, Lanna E. B.; Souza, Felipe M.; Pinheiro, Victor S.; Moura, João P. C.; Trench, Aline B.; de Almeida, James M.; Autreto, Pedro A. S.; Lanza, Marcos R. V.; Santos, Mauro C.
Sodium niobate microcubes decorated with ceria nanorods for hydrogen peroxide electrogeneration: An experimental and theoretical study Journal Article
Em: Journal of Alloys and Compounds, vol. 965, 2023, ISSN: 0925-8388.
Links | BibTeX
@article{Antonin2023,
title = {Sodium niobate microcubes decorated with ceria nanorods for hydrogen peroxide electrogeneration: An experimental and theoretical study},
author = {Vanessa S. Antonin and Lanna E. B. Lucchetti and Felipe M. Souza and Victor S. Pinheiro and João P.C. Moura and Aline B. Trench and James M. de Almeida and Pedro A. S. Autreto and Marcos R.V. Lanza and Mauro C. Santos},
doi = {10.1016/j.jallcom.2023.171363},
issn = {0925-8388},
year = {2023},
date = {2023-07-14},
urldate = {2023-11-00},
journal = {Journal of Alloys and Compounds},
volume = {965},
publisher = {Elsevier BV},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
doi:10.1016/j.jallcom.2023.171363
Fechar
Lucchetti, Lanna E. B.; Autreto, Pedro A. S.; de Almeida, James M.; Santos, Mauro C.; Siahrostami, Samira
Unravelling catalytic activity trends in ceria surfaces toward the oxygen reduction and water oxidation reactions Journal Article
Em: React. Chem. Eng., vol. 8, não 6, pp. 1285–1293, 2023, ISSN: 2058-9883.
Resumo | Links | BibTeX
@article{Lucchetti2023,
title = {Unravelling catalytic activity trends in ceria surfaces toward the oxygen reduction and water oxidation reactions},
author = {Lanna E. B. Lucchetti and Pedro A. S. Autreto and James M. de Almeida and Mauro C. Santos and Samira Siahrostami},
doi = {10.1039/d3re00027c},
issn = {2058-9883},
year = {2023},
date = {2023-05-30},
journal = {React. Chem. Eng.},
volume = {8},
number = {6},
pages = {1285--1293},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {Different facets of ceria exhibit activities for the entire spectrum of oxygen electrochemistry.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Different facets of ceria exhibit activities for the entire spectrum of oxygen electrochemistry.
Fechar
doi:10.1039/d3re00027c
Fechar
de Oliveira, Caique Campos; Medina, Matheus; Galvao, Douglas S.; Autreto, Pedro A. S.
Tetra-penta-deca-hexagonal-graphene (TPDH-graphene) hydrogenation patterns: dynamics and electronic structure Journal Article
Em: Phys. Chem. Chem. Phys., vol. 25, não 18, pp. 13088–13093, 2023, ISSN: 1463-9084.
Resumo | Links | BibTeX
@article{Oliveira2023b,
title = {Tetra-penta-deca-hexagonal-graphene (TPDH-graphene) hydrogenation patterns: dynamics and electronic structure},
author = {Caique Campos de Oliveira and Matheus Medina and Douglas S. Galvao and Pedro A. S. Autreto},
doi = {10.1039/d3cp00186e},
issn = {1463-9084},
year = {2023},
date = {2023-05-10},
urldate = {2023-05-10},
journal = {Phys. Chem. Chem. Phys.},
volume = {25},
number = {18},
pages = {13088--13093},
publisher = {Royal Society of Chemistry (RSC)},
abstract = {Fully atomistic molecular dynamics and density functional theory of hydrogenation process on 2D carbon allotrope: tetra-penta-deca-hexagonal graphene.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Fully atomistic molecular dynamics and density functional theory of hydrogenation process on 2D carbon allotrope: tetra-penta-deca-hexagonal graphene.
Fechar
doi:10.1039/d3cp00186e
Fechar
de Oliveira, Caique Campos; Autreto, Pedro A. S.
Optimized 2D nanostructures for catalysis of hydrogen evolution reactions Journal Article
Em: MRS Advances, vol. 8, não 6, pp. 307–310, 2023, ISSN: 2059-8521.
Resumo | Links | BibTeX
@article{Oliveira2023,
title = {Optimized 2D nanostructures for catalysis of hydrogen evolution reactions},
author = {Caique Campos de Oliveira and Pedro A. S. Autreto},
url = {https://link.springer.com/article/10.1557/s43580-023-00549-7},
doi = {10.1557/s43580-023-00549-7},
issn = {2059-8521},
year = {2023},
date = {2023-03-27},
urldate = {2023-06-00},
journal = {MRS Advances},
volume = {8},
number = {6},
pages = {307--310},
publisher = {Springer Science and Business Media LLC},
abstract = {Electrochemical water splitting can produce hydrogen without harmful emissions. However, the need for more cheap and efficient catalysts presents a significant bottleneck for this technology. With a diverse chemical composition and electronic properties, transition metal dichalcogenides have been extensively investigated for catalysing hydrogen evolution reactions. Major approaches to enhance these materials’ activity are based on increasing active site counting and enhancing their intrinsic activity, which can be achieved by doping. In this work, we performed ab initio calculations to investigate the catalytic activity of pristine and Pt-doped 1 T-TiSe2. Our results show that basal plane transition metal sites are meta-stable for adsorption, while chalcogen sites are most favourable. Furthermore, catalytic activity was enhanced after the Pt introduction, as indicated by the change in the ∆G towards zero. Nonetheless, Pt sites exhibited the best activity among the investigated sites. },
keywords = {},
pubstate = {published},
tppubtype = {article}
}

Fechar
Electrochemical water splitting can produce hydrogen without harmful emissions. However, the need for more cheap and efficient catalysts presents a significant bottleneck for this technology. With a diverse chemical composition and electronic properties, transition metal dichalcogenides have been extensively investigated for catalysing hydrogen evolution reactions. Major approaches to enhance these materials’ activity are based on increasing active site counting and enhancing their intrinsic activity, which can be achieved by doping. In this work, we performed ab initio calculations to investigate the catalytic activity of pristine and Pt-doped 1 T-TiSe2. Our results show that basal plane transition metal sites are meta-stable for adsorption, while chalcogen sites are most favourable. Furthermore, catalytic activity was enhanced after the Pt introduction, as indicated by the change in the ∆G towards zero. Nonetheless, Pt sites exhibited the best activity among the investigated sites.
Fechar
https://link.springer.com/article/10.1557/s43580-023-00549-7
doi:10.1557/s43580-023-00549-7
Fechar

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