Article
Physics, Applied
Mingming Yan, Tianchong Zhang, Bo Wang, Jing Liu, Xiaoxiao Liang, Yuanze Xu, Futing Yi
Summary: The study observed the evolution of Pt coverage on different surfaces based on experimental results, revealing the importance of chemisorption, metal atom diffusion, and up-stepping in film growth. Pt films were easier to form on Al2O3 and Ni surfaces compared with on Si and Au surfaces.
JOURNAL OF APPLIED PHYSICS
(2021)
Article
Energy & Fuels
Yating Zhang, Wei Liu, Youyu Zhu, Yongling Zhang, Ruizhe Zhang, Keke Li, Guoyang Liu
Summary: The novel CuO/Cu2O/coal-based reduced graphene oxide nanosheet composite shows higher reversible capacity and stability, making it a potential candidate for high-rate lithium-ion battery anode materials.
Article
Nanoscience & Nanotechnology
Alberto S. de Leon, Maria de la Mata, Ivan R. Sanchez-Alarcon, Rafael Abargues, Sergio I. Molina
Summary: In this work, a series of porous CsPbBr3 nanocrystals as light emitters were prepared using the breath figure approach. Microscopy analysis showed that the nanocrystals were evenly distributed within the polymer matrix but mainly confined inside the pores. The CsPbBr3 nanocrystals maintained their optical properties after film formation, indicating their stability inside the polystyrene matrix. The high porosity and defined micropatterning of the surfaces resulted in highly hydrophobic behavior, making them self-cleaning.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Review
Polymer Science
Ottavia Bellotto, Maria C. Cringoli, Siglinda Perathoner, Paolo Fornasiero, Silvia Marchesan
Summary: The use of peptides as templates for inorganic nanoparticle formation is an environmentally friendly method with applications in various fields. Short-peptide gelators provide dynamic supramolecular environments, and recent research progress outlines future research directions.
Article
Chemistry, Multidisciplinary
Dor Zaguri, Manuela R. Zimmermann, Georg Meisl, Aviad Levin, Sigal Rencus-Lazar, Tuomas P. J. Knowles, Ehud Gazit
Summary: The study found that the aggregation propensity of three phenylalanine-containing molecules increases significantly with size, with triphenylalanine being the most aggregation-prone species under experimental conditions. In the context of classical nucleation theory, this increase in aggregation propensity is attributed to the larger free energy decrease upon aggregation of larger peptides, and not to the presence/absence of a peptide bond per se. This work provides insights into the aggregation processes of chemically simple systems and suggests that both backbone-containing peptides and backbone-lacking amino acids assemble through a similar mechanism, supporting the classification of amino acids in the continuum of amyloid-forming building blocks.
Article
Multidisciplinary Sciences
Alexander Hensley, William M. Jacobs, W. Benjamin Rogers
Summary: DNA-coated colloids can self-assemble into various crystal structures, and we have used microfluidics to quantify the kinetics of crystallization. Our study shows that classical theories can accurately predict nucleation and growth rates, and we have successfully designed large single crystals with specific structural coloration.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Review
Chemistry, Multidisciplinary
Buzuayehu Abebe, Dereje Tsegaye, H. C. Ananda Murthy
Summary: The synthesis of nanoscale materials using nanotechnology has attracted the attention of scientists. In the bottom-up approach, atoms aggregate to form nuclei, which then undergo further growth. Real-time liquid phase analysis can be used to control the formation process of nanocrystals. Solution combustion synthesis is an efficient method for producing porous materials and can also be used to synthesize doped and hybrid nanomaterials. Additionally, kinetic and thermodynamics controlled architecture-directing agent-assisted SCS can form colloidal nanocrystal frameworks, which have broad applications in energy devices.
Article
Chemistry, Inorganic & Nuclear
Stamatis S. Passadis, Sofia Hadjithoma, Michael G. Papanikolaou, Anastasios D. Keramidas, Haralampos N. Miras, Themistoklis A. Kabanos
Summary: The hydrolytically stable dioxime ligand, H(3)pidiox, exhibits strong chelation with hard metals in high oxidation states, potentially useful in metal sequestering processes from aqueous solutions. Experimental data analysis indicates that zirconium compounds with different structural features can be synthesized under different pH conditions.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Luying Song, Biao Yang, Xing Fan, Yahui Mao, Huan Shan, Junbo Wang, Kaifeng Niu, Zhengming Hao, Zhiwen Zeng, Youyong Li, Aidi Zhao, Haiping Lin, Lifeng Chi, Qing Li
Summary: In this study, large-scale self-assembly of atomically precise organometallic supramolecules was achieved through cascaded on-surface chemical reactions and intermolecular interactions. Supramolecules with defined size and shape were built through intramolecular reactions and intermolecular metal coordination, followed by the formation of ordered two-dimensional arrays with the assistance of Br atoms. The mechanism of this process was investigated from the perspectives of thermodynamics and kinetics.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Luying Song, Biao Yang, Xing Fan, Yahui Mao, Huan Shan, Junbo Wang, Kaifeng Niu, Zhengming Hao, Zhiwen Zeng, Youyong Li, Aidi Zhao, Haiping Lin, Lifeng Chi, Qing Li
Summary: This study demonstrates the self-organization of atomically precise organometallic supramolecules through cascaded on-surface chemical reactions. The combination of intra- and inter-supramolecular interactions allows for the construction of supramolecules with defined size and shape. With the assistance of C-H···Br interactions, well-ordered two-dimensional arrays can be formed. This research is important for understanding and exploring the mechanism of self-assembled supramolecules.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Review
Chemistry, Multidisciplinary
Sunghee Lee, Kyunjong Sim, So Yoon Moon, Jisu Choi, Yoojung Jeon, Jwa-Min Nam, So-Jung Park
Summary: The spatial arrangement of plasmonic nanoparticles can significantly affect their interaction with electromagnetic waves and control their optical properties. Recent advances in bottom-up chemical strategies have enabled precise control over the assembly structure of metal nanoparticles, leading to the construction of smart dynamic nanostructures capable of reversible structural changes.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Li-Yun Su, Hsin-Hsiang Huang, Yan-Cheng Lin, Guan-Lin Chen, Wen-Chang Chen, Wei Chen, Leeyih Wang, Chu-Chen Chueh
Summary: In this study, interfacial engineering using an amphiphilic dendritic block copolymer (DBC) and gold nanoparticles (NPs) was demonstrated to enhance the performance and thermal stability of non-fullerene bulk-heterojunction organic photovoltaic devices. The newly developed DBC@AuNPs interlayer improved device efficiency by enabling better energy-level alignment and enhanced interfacial compatibility at the ZnO/BHJ interface, showing great potential for commercialization with a T(80)lifetime of over 1.79 years at room temperature.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Fengdong Qu, Shendan Zhang, Chaozhu Huang, Xuyun Guo, Ye Zhu, Tiju Thomas, Haichuan Guo, J. Paul Attfield, Minghui Yang
Summary: This study presents a general strategy to overcome water-sensitivity issues in semiconducting metal oxides (SMOXs) by coating them with a hydrophobic polymer separated by a metal-organic framework (MOF) layer. Sensors using these nanoparticles show near-constant responses across a wide humidity range, with notable performance below 20% RH. Selectivity enhancement and humidity-independent sensitivity are achieved, leading to improved humidity-resistant gas sensors.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Hossein Eslami, Florian Mueller-Plathe
Summary: The self-assembly of triblock Janus particles and the relative stability of different lattices were simulated. The nucleation process consists of two steps: the formation of a compact and disordered liquid cluster, followed by the reorientation of particles to form crystalline nuclei. The nucleation barriers for pyrochlore and perovskite were similar to previously studied 2D kagome lattices, while the barrier for diamond was larger.
Article
Materials Science, Ceramics
Jingye Qian, Xuejiao Li, Tingzhao Zhang, Xiande Dai, Zhixiong Bi, Kai Rong
Summary: A new method for the synthesis of tricobalt tetraoxide (Co3O4) nanoparticles was proposed in this study. By using the emulsion detonation method, the precursor cobalt nitrate hexahydrate (Co(NO3)2•6H2O) was uniformly dispersed in the explosives. The synthesized Co3O4 nanoparticles had high purity and mainly consisted of sphere-like particles with a size of approximately 50 nm. This method could provide a new approach for the low-cost production of Co3O4 nanoparticles.
CERAMICS INTERNATIONAL
(2023)
Article
Chemistry, Physical
Farahnaz Maleki, Gianfranco Pacchioni
Summary: This work investigates the effect of iso-valent dopants on the chemical reactivity of the SnO2 (110) surface. The results show that surface or sub-surface sites are preferred over bulk ones. It is found that SnO2 exhibits higher reactivity in all reaction steps of formic acid decomposition compared to rutile TiO2 (110) with the same structure and morphology.
Article
Chemistry, Physical
Giovanni Di Liberto, Luis A. Cipriano, Gianfranco Pacchioni
Summary: One of the objectives of electronic structure theory is to predict chemical and catalytic activities, which has become less complex with the use of single atom catalysts and graphene-based catalysts for electrocatalytic reactions. The rapid growth of theoretical studies based on density functional theory (DFT) and proposals of universal descriptors have provided guidance for the synthesis of efficient catalysts. However, there are still challenges in predicting catalyst activity, such as the accuracy of calculations, neglect of important contributions, and the physical meaning of proposed descriptors, not to mention reproducibility issues.
Article
Chemistry, Physical
Giovanni Di Liberto, Luis A. Cipriano, Gianfranco Pacchioni
Summary: This article investigates the relationship between metal atoms and their surrounding environment in single atom catalysts (SACs). The numerical experiments reveal that changing the active site or the surrounding environment can lead to significant variations in catalytic activity. The implications of this conclusion for modeling studies of SACs are discussed.
Article
Multidisciplinary Sciences
Ilaria Barlocco, Luis A. Cipriano, Giovanni Di Liberto, Gianfranco Pacchioni
Summary: This study investigates the impact of different exchange-correlation functionals on the catalytic activity of single atom catalysts in hydrogen and oxygen evolution reactions. The results show that the choice of functional can lead to significant deviations in the predicted activity for different transition metals.
ADVANCED THEORY AND SIMULATIONS
(2023)
Article
Chemistry, Physical
Giovanni Di Liberto, Sergio Tosoni
Summary: We investigated the interface between carbon nitride (C3N4) and phosphorene nanosheets (P-ene) using Density Functional Theory (DFT) calculations. The formation of the interface is driven by Van der Waals forces. The thickness of P-ene nanosheets determines the band edges offsets and the separation of charge carriers. The system transitions from a nearly type-II to a type-I junction as the thickness of P-ene increases.
Review
Chemistry, Physical
Sergio Tosoni, Giovanni Di Liberto, Ivana Matanovic, Gianfranco Pacchioni
Summary: In this tutorial review, the state-of-the-art modeling approaches of Single Atom Catalysts (SAC) for water splitting and fuel cells reactions are reported. The discussion focuses on Hydrogen Evolution Reaction (HER), Oxygen Reduction Reaction (OER), Hydrogen Oxidation Reaction (HOR), and Oxygen Reduction Reaction (ORR). The aim is to emphasize the relevant aspects of SACs modeling and provide guidance for computational chemists and experimentalists. The review covers methodologies, prediction of electronic properties, validation of structural models, prediction of catalytic activity and selectivity, and analysis of current challenges and limitations.
JOURNAL OF POWER SOURCES
(2023)
Article
Nanoscience & Nanotechnology
Farahnaz Maleki, Giovanni Di Liberto, Gianfranco Pacchioni
Summary: In this work, the pH- and facet-dependent surface chemistry of TiO2/water interfaces was studied using ab initio molecular dynamics simulations. Acid-base equilibrium constants were determined at the interface, allowing for estimation of the pH at the point of zero charge, an important experimental observable. The amount of H+, OH-, and adsorbed H2O species on the surfaces was predicted based on simulated equilibrium constants, providing insights into water splitting semi-reactions. The complex morphology of TiO2 particles was approximated by considering different surfaces.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Sergio Tosoni
Summary: Mn3O4 Hausmannite thin films supported on (Cu, Ag, Au) coinage metals were investigated using DFT calculations. The interface between the films and metal support exhibited different lattice and ionic match, leading to different interactions. The films on Cu (111) and Au (111) weakly adhered due to unfavorable structural match, while strong adhesion was observed on Ag(100) with commensurate lattice and epitaxial growth. A negative charge flow from the support to the film was reported, resulting in the reduction of the film and an increase in magnetic moments of metal ions in the octahedral sublattice. The ferrimagnetic ordering varied in supported films exposing different crystal faces.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Alexander Fuhrich, Joachim Paier, Sergio Tosoni, Adrian Leandro Lewandowski, Leonard Gura, Wolf-Dieter Schneider, Gianfranco Pacchioni, Hans-Joachim Freund
Summary: Two-dimensional oxide films, including silica, germania, and mixed silica-germania films, supported on a Ru(0001) single crystal surface were studied. The modification of the properties of silica films through the incorporation of germanium atoms was investigated. X-ray photoelectron spectroscopy in combination with LEED and I/V LEEM measurements were used to judge the formation of mixed films.
ISRAEL JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Tilak Das, Sergio Tosoni
Summary: A self-consistent Hubbard-U search was conducted on the bulk honeycomb layered oxide SrRu2O6 for potential applications as Li and post-Li battery cathode materials. The study employed first-principles density functional theory (DFT) based calculations and analysis. The results revealed that intercalation of Li, Ca, and Al metals did not affect the SRO magnetic ordering. The host SRO showed a quenched magnetic moment after intercalation, indicating the transfer of electrons to neighboring Ru sublattices.
SOLID STATE IONICS
(2023)
Review
Chemistry, Physical
Giovanni Di Liberto, Ilaria Barlocco, Livia Giordano, Sergio Tosoni, Gianfranco Pacchioni
Summary: This article discusses several fundamental elements required for successful computational modeling of single-atom catalysts (SACs) for electrocatalytic applications, including the role of the adopted exchange-correlation functional within a given DFT approach and the role of the local coordination of the active transition metal atom. Next, it explores new intermediates that can form on SACs, which are not present on extended metal electrodes, and how to model solvation, with a focus on the dual role of water as both a solvent and a ligand on SACs. Finally, challenges related to the inclusion of pH and voltage in models and some open issues concerning the rational design of new SACs are discussed.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Physical
Ilaria Barlocco, Giovanni Di Liberto, Gianfranco Pacchioni
Summary: Single Atom Catalysts (SACs) bridge the gap between homogenous and heterogenous catalysis and show promise in various chemical reactions, including water splitting. This study focuses on SACs embedded in Covalent Organic Frameworks (COFs) and investigates their reactivity in Hydrogen and Oxygen Evolution Reactions (HER and OER, respectively) using density functional theory (DFT). The results reveal the formation of unique intermediates and shed light on the reaction mechanism, providing valuable insights for the design of novel catalytic materials.
Article
Chemistry, Multidisciplinary
Giovanni Di Liberto, Sergio Tosoni, Luis A. Cipriano, Gianfranco Pacchioni
Summary: Single-atom catalysis is a highly investigated topic in the catalytic community, offering advantages such as the use of minimal precious metals, higher selectivity, and bridging homogeneous and heterogeneous catalysis. The combination of advanced characterization techniques and theoretical calculations can provide a conceptual framework to better understand structure-function relationships.
ACCOUNTS OF MATERIALS RESEARCH
(2022)
Article
Chemistry, Multidisciplinary
Saeed Sovizi, Sergio Tosoni, Robert Szoszkiewicz
Summary: Sub-nanometer MoOx clusters were found on the basal planes of 2H MoS2 crystals during thermal oxidative etching at 370 degrees C. These clusters were predominantly composed of single MoO3 molecules and their dimers at sulfur vacancies, as observed using high resolution non-contact atomic force microscopy. Additional spectroscopic and microscopy techniques confirmed the sparse coverage of MoO3/MoOx species on the MoS2 surface. The findings support the previously proposed stoichiometry of oxidative etching.
NANOSCALE ADVANCES
(2022)
