Article
Chemistry, Physical
Peng Wang, Thomas P. Senftle
Summary: Identifying catalysts for non-oxidative propane dehydrogenation is crucial due to the increasing demand for propylene. Recent experimental work has shown that earth-abundant metals like iron exhibit good performance in PDH. Carbon-rich surfaces show higher selectivity for propylene production compared to iron-rich surfaces.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Inorganic & Nuclear
Xia-Ping Lei, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Chang-Ming Nie, Wei-Qun Shi
Summary: Separation of trivalent actinide and lanthanide is a major challenge in nuclear waste treatment. Recent research has shown that ligands modified with amide groups have excellent separation performance. The present study investigates the extraction behaviors of Am(III) and Eu(III) using different ligands with varying levels of preorganization. The results demonstrate that ligands with a completely preorganized structure exhibit the strongest extraction ability and highest selectivity, while those with a more flexible skeleton have weaker extraction ability and lower selectivity. This study provides valuable information for designing efficient ligands for An(III)/Ln(III) separation using a preorganization strategy.
DALTON TRANSACTIONS
(2022)
Review
Immunology
Wenjing Chen, Yuxue Cao, Yuanyuan Zhong, Jing Sun, Jingcheng Dong
Summary: CD4(+) helper T cell subsets play a critical role in the pathogenesis of asthma. Different subsets of Th cells differentiate under the stimulation of different cytokines and are driven by lineage-specific transcription factors. The balance between effector Th cell response and Treg cell immunosuppression is essential for maintaining immune homeostasis and understanding the immunopathological mechanism of asthma. Recent studies have found that certain factors involved in effector Th cell response also contribute to the development and function of Treg cells. This review aims to summarize the role of these factors in Treg cell development and function to gain new insights into the immunopathological mechanism and potential therapy strategies of asthma.
FRONTIERS IN IMMUNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Zi-Rong Ye, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Hong-Qing Wang, Wei-Qun Shi
Summary: Designing ligands with efficient actinide/lanthanide separation performance is crucial for the disposal of radioactive waste and the recovery of minor actinides. This study investigated the selective back-extraction of Am(III) over Eu(III) using hydrophilic hydroxylated triazolyl-based ligands. The results showed that Am-N bonds have more covalent character compared to Eu-N bonds. The ligand with the best selectivity for Am(III)/Eu(III) was found to have the largest difference in covalency between Am-N and Eu-N bonds.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Xiao-Bo Li, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Meng Zhang, Zhi-Fang Chai, Wei-Qun Shi
Summary: This study focuses on the reduction mechanism of neptunium with phenylhydrazine, revealing that phenylhydrazine has better reduction ability to Np(VI). The research elucidates the bonding evolution for the structures of the reaction pathways.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Inorganic & Nuclear
Francesco Galluccio, Elena Macerata, Patrik Wessling, Christian Adam, Eros Mossini, Walter Panzeri, Mario Mariani, Andrea Mele, Andreas Geist, Petra J. Panak
Summary: The challenging issue of spent nuclear fuel management is being addressed through the development of advanced technologies, such as the use of selective lipophilic ligands. These ligands have shown promising results in safer reprocessing of nuclear fuel and reducing environmental impact.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Zheng-Qing Huang, You-Tao Chen, Chun-Ran Chang, Jun Li
Summary: This study reports three dual-metal-site catalysts based on nitrogen-doped graphene for the nonoxidative coupling of methane to C-2 hydrocarbons. Among them, Co-2-N-C exhibits the best catalytic activity and selectivity. Microkinetic modeling and electronic structure analysis demonstrate the high-temperature stability and coke resistance of the catalyst.
Article
Chemistry, Multidisciplinary
Neubi F. F. Xavier Jr, Anthony J. R. Payne, Glauco F. Bauerfeldt, Marco Sacchi
Summary: The viability of catalytic methane decomposition (CMD) on carbon-based materials, specifically graphene nanoribbons, was investigated. The bare carbon edges of graphene nanoribbons were found to exhibit comparable performance to commonly used metallic and bi-metallic catalysts for methane decomposition.
FRONTIERS IN CHEMISTRY
(2023)
Review
Chemistry, Inorganic & Nuclear
Umit B. Demirci
Summary: Ammonia borane (AB) was discovered in the 1950s, but its potential as a chemical hydrogen storage material was only recognized in the 2000s. It has complex decomposition mechanisms, with recent studies providing insights into the process and potential strategies for destabilization to release pure hydrogen. This understanding is crucial for technological progress in utilizing AB for hydrogen storage.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Biochemistry & Molecular Biology
Stefano Borocci, Felice Grandinetti, Nico Sanna
Summary: In this study, the structure, stability, and bonding situation of noble gas-silicon cations were investigated using theoretical calculations. The results show that the Ng-Si bonds are generally tight and have a partial covalent character. The degree of Ng-Si interaction in NgSiX(3)(+) is influenced by the polarizability of Ng and the Lewis acidity of SiX3+. Peculiar effects related to the small size of He were observed in HeSiX3+. The Ng-Si interaction in NgSiF(2)(2+) increases with the increased charge on Si, and the bond strength also increases in the inserted FNgSiF(2)(+) due to the cooperative effect of the adjacent F atom. On the other hand, the ligation of a second Ar atom to ArSiX3+ weakens the bond.
Article
Chemistry, Inorganic & Nuclear
Yao Zou, Jian-Hui Lan, Li-Yong Yuan, Cong-Zhi Wang, Qun-Yan Wu, Zhi-Fang Chai, Peng Ren, Wei-Qun Shi
Summary: In this study, four hydrophilic sulfonated and phosphorylated ligands L1, L2, L3, and L4 based on the bipyridine and phenanthroline backbones were designed, and their structures, neutral complexes [ML(NO3)3] (M = Am, Eu), and thermodynamic properties of complexing reactions were studied through density functional theory. According to the changes of the Gibbs free energy for the back-extraction reactions, the phenanthroline-based ligands L2 and L4 showed stronger complexing capacity for both Am(III) and Eu(III) ions, while the phosphorylated ligand L3 with the bipyridine framework exhibited the highest Am(III)/Eu(III) selectivity. This study provides theoretical insights into the separation of actinide(III)/lanthanide(III) using hydrophilic sulfonated and phosphorylated N-donor ligands.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Zhexi Lin, Shizhong Liu, Steven R. Denny, William N. Porter, Stavros Caratzoulas, J. Anibal Boscoboinik, Dionisios G. Vlachos, Jingguang G. Chen
Summary: The study investigated the active sites of WOx/Pt model surfaces using carbon monoxide and isopropyl alcohol as probe molecules, identifying two distinct active sites responsible for different reaction pathways. Various experimental techniques and computational methods were combined to provide insights into the design of relevant catalysts for the catalytic upgrading of biomass-derived oxygenates.
Article
Chemistry, Inorganic & Nuclear
Zi-Rong Ye, Qun-Yan Wu, Cong-Zhi Wang, Jian-Hui Lan, Zhi-Fang Chai, Hong-Qing Wang, Wei-Qun Shi
Summary: This study focused on the separation of Am(III)/Eu(III) using four hydrophilic sulfonated ligands based on the phenanthroline and bipyridine framework. The tetrasulfonated ligand with a bipyridine framework showed the strongest complexing ability for metal ions, while the disulfonated ligand exhibited the highest selectivity for Am(III)/Eu(III). Thermodynamic analysis confirmed the selectivity of the hydrophilic sulfonated ligands towards Am(III) over Eu(III). Compared to hydrophobic nonsulfonated ligands, these hydrophilic sulfonated ligands demonstrated better complexing ability and selectivity for Am(III)/Eu(III) separation.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Jiayu Huang, Brian K. Kendrick, Dong H. Zhang
Summary: Ultracold chemical reactions involve collisions at temperatures near absolute zero, which can lead to significant reactivity in molecular systems with barrierless and exoergic reaction pathways. The study reveals that the geometric phase can significantly alter the outcome of ultracold reactions, and quantum control techniques may be effective in controlling reactivity.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Inorganic & Nuclear
Liuting Zhang, Yan Zhang, Fuying Wu, Yiqun Jiang, Yijing Wang
Summary: Amorphous NiCoB nanoparticles were synthesized and used as high-activity catalysts to improve the hydrogen storage properties of MgH2. The MgH2-NiCoB composite absorbed 3.6 wt % H2 at 85 degrees C and released 5.5 wt % H2 below 270 degrees C within 600 s. Microstructure analysis revealed the generation of active ingredients at the surface of NiCoB, facilitating hydrogen diffusion and decreasing kinetic barriers.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Maicon Pierre Lourenco, Egon Campos dos Santos, Lars G. M. Pettersson, Helio Anderson Duarte
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2020)
Article
Chemistry, Physical
Fernando Steffler, Guilherme Ferreira De Lima, Helio Anderson Duarte
JOURNAL OF MOLECULAR STRUCTURE
(2020)
Article
Chemistry, Inorganic & Nuclear
Alexandre C. Bertoli, Ana Gabriella C. Miguita, Raquel M. Mingote, Rodinei Augusti, Helio A. Duarte
Summary: In this study, PSI-MS combined with DFT calculations was used to analyze the distribution of hafnium and zirconium species in an aqueous acid solution with NO3- and F- anions, revealing their stability and coordination modes. It was found that Zr(IV) fluoroanions exhibited high electron affinity in the gas phase, showing consistent thermodynamic stability in experimental and computational results. The presence of fluoride and nitrate led to the formation of dimers with mu(2)-F bridges, highlighting the importance of studying cationic metals in aqueous environments for future research.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Walber Goncalves Guimaraes, Guilherme Ferreira de Lima, Helio Anderson Duarte
Summary: This study investigated the surface properties of materials such as Goethite and diaspore through calculations and comparisons, revealing differences in surface reactivity that are significant for geochemical processes.
Article
Chemistry, Physical
Paulo Roberto Garces Goncalves Jr, Heitor Avelino De Abreu, Helio Anderson Duarte
Summary: This study investigates the adsorption mechanism and oxidation process of arsenite and arsenate on hausmannite surfaces using computational methods. Different adsorption sites and the presence of water are found to have a significant impact on the reaction. The findings are important for mitigating the environmental impact of arsenic-rich tailings.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Beatriz Lobo Filgueiras de Miranda Gomes, Alexandre C. Bertoli, Helio A. Duarte
Summary: This study investigates the effect of pH value on the formation of polysulfide chains and the formation of elemental sulfur through electronic structure calculations. The results show that species with lower protonation levels are more favorable for the formation of polysulfide chains and elemental sulfur.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Biochemistry & Molecular Biology
Selma Fabiana Bazan, Helio Anderson Duarte, Guilherme Ferreira de Lima
Summary: DFT calculations were used to study the adsorption of O-2 and [Fe(H2O)(2)(OH)(3)] molecules on the surfaces of CuFeS2. The results showed that O-2 molecule strongly adsorbs on the (001) surface through a dissociative pathway, while [Fe(H2O)(2)(OH)(3)] molecule undergoes a bidantade coordination adsorption. The adsorption behaviors on the (112) surface were weaker compared to the (001) surface.
JOURNAL OF MOLECULAR MODELING
(2022)
Article
Chemistry, Physical
Walber Goncalves Guimaraes Jr, Guilherme Ferreira de Lima, Helio Anderson Duarte
Summary: Ferrihydrite (Fh) is an important oxy-hydroxide that plays significant roles in geochemistry, ion mobility, adsorption, and the formation of more crystalline phases. This study proposes a chemical model for the substitution of Fe sites by Al in Fh. DFT/plane wave calculations reveal the local environment and investigate the structural and electronic properties of Al-substituted Fh. The results show that Al prefers to replace the octahedral Fe sites and affect various parameters such as NMR and Moessbauer parameters.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Metallurgy & Metallurgical Engineering
Walber Goncalves Guimaraes Jr, Guilherme Ferreira de Lima, Helio Anderson Duarte
Summary: Hematite (Hem) and Goethite (Goe) are the most abundant iron oxides in the natural environment. Al-substituted Hem and Goe have been studied for their structural and thermodynamic properties using Density Functional calculations. The substitution is found to be a local phenomenon and is independent of the degree of substitution reached. The formation of Al-bearing systems is energetically less favored compared to pristine Goe and Hem.
Article
Chemistry, Physical
Walber Goncalves Guimaraes Jr, Guilherme Ferreira de Lima, Helio Anderson Duarte
Summary: A chemical model for the isomorphic substitution of Al in poorly crystalline oxyhydroxide Ferrihydrite (Fh) has been proposed. Using DFT/plane wave calculations, it was found that Al prefers to replace the octahedral Fe sites. The substitution of Al affects the quadrupolar coupling constant of Al-27 NMR and Mo''ssbauer quadrupole splitting and isomer shift parameters, which are influenced by the concentration of substituted sites. Additionally, Al substitution increases the band gap dispersion and the formation of Al electronic states in the conduction band. The standard Helmholtz free energy of Al substitution has also been estimated and discussed in detail.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Engineering, Environmental
Gabriela Cordeiro Silva, Alexandre Carvalho Bertoli, Helio Anderson Duarte, Ana Claudia Queiroz Ladeira
Summary: The ion exchange process for the recovery of rare earth elements from acid waters was studied using experimental and theoretical approaches. The results showed that La had a higher preference than Y during the loading experiments, and approximately 80% of the adsorbed REE could be eluted using a CaCl2 solution. DFT calculations indicated that the functional group in the cation exchange resin acted as a complexing agent.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Guilherme Ferreira de Lima, Selma Fabiana Bazan, Heitor Avelino de Abreu, Hello Anderson Duarte
Summary: A comprehensive understanding of geochemical, environmental, and physical chemical phenomena is crucial in seeking sustainable solutions for mining activities. The oxidation process of non-ferrous metal ores poses a significant environmental hazard known as Acid Mine Drainage (AMD). However, the surface phenomenon and the mineral - aqueous solution interfaces are not fully understood yet, emphasizing the importance of further research for sustainable mining.
REVISTA VIRTUAL DE QUIMICA
(2022)
Article
Chemistry, Multidisciplinary
Angela L. Andrade, Thais D. Cardoso, Sergio S. Thomasi, Meiry E. Alvarenga, Mirra A. N. da Silva, Elisangela J. Magalhaes, Helio A. Duarte, Katia J. de Almeida
Summary: A novel method was developed for simultaneous quantification of L-dopa and C-dopa in pharmaceutical preparations by investigating the oxidation process of these drugs experimentally and theoretically, based on DFT. The method showed good linearity, precision, and accuracy, providing a promising alternative for quality control analysis of the Parkinson's disease pharmaceutical preparation.
Article
Chemistry, Multidisciplinary
Helio A. Duarte
Article
Engineering, Environmental
Alexandre Carvalho Bertoli, Matheus Campos Quintao, Heitor Avelino De Abreu, Ana Claudia Queiroz Ladeira, Helio Anderson Duarte
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2019)