Article
Materials Science, Multidisciplinary
Emile Haurat, Jean-Paul Crocombette, Marc Tupin
Summary: Using Density Functional Theory, the interactions of hydrogen atoms with point defects in monoclinic zirconia were calculated. The substitution of Zr atoms by Nb and Sn, as well as oxygen vacancies, were considered. Various charges for the complexes formed by hydrogen atoms and the defects were examined. The findings showed little interaction between H and Sn atoms, weak binding between H and Nb atoms, and strong binding between hydrogen atoms and oxygen vacancies. The stable form of hydrogen was observed to vary with the Fermi level in zirconia, and the concentrations of different forms of hydrogen were calculated using a thermodynamical model. The study provided insights into the variation of hydrogen diffusion coefficient through the oxide layer in zirconia.
Article
Chemistry, Multidisciplinary
Nicolaj Inunnguaq Jessen, Joseph A. Izzo, Marek S. Modlinski, Giulio Bertuzzi, Karl Anker Jorgensen
Summary: The development of higher-order cycloadditions has been limited due to the need for highly conjugated and reactive pi-systems. Recent research shows that organocatalysis can be an efficient mediator to overcome these challenges. Computational studies have also found that the impact of benzofusions on higher-order cycloadditions can be explained by changes in energy barriers.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Susana Portela, Israel Fernandez
Summary: The poorly understood factors governing the small molecule activation reactions mediated by diazaborinines have been computationally explored in detail using quantum chemical tools. This study investigates the activation of E-H sigma-bonds (E = H, C, Si, N, P, O, S) and reveals their exergonic nature and relatively low activation barriers. The reactivity trend, as well as the mode of action of the diazaborinine system, are analyzed quantitatively using the activation strain model and energy decomposition analysis method.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Nitul S. Rajput, Hionsuck Baik, Jin-You Lu, Srinivasa Reddy Tamalampudi, Raman Sankar, Amal Al Ghaferi, Matteo Chiesa
Summary: The study reveals the unique complexity of the quasi-periodic structure of SnTiS3 misfit compound using advanced electron microscopy techniques. It provides important insights for designing nanoengineered heterojunction compound devices or for theoretical studies.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Yuanmin Zhu, Ping Liao, Wandong Xing, Jiayu Liu, Jizhe Cui, Cai Jin, Lang Chen, Biao Wang, Rong Yu
Summary: This study systematically investigates the atomic structure, chemical distribution and electronic structure of RP faults in perovskite LaNiO3 using STEM and DFT calculations. The study reveals fluctuations in oxygen content and mixed valence of Ni cations at RP faults.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Diego Cortes-Arriagada, Sebastian Miranda-Rojas, Francisca Cid-Mora, Alejandro Toro-Labbe
Summary: Phosphorene and MN4 compounds can form stable hybrid nanostructures with non-degenerated adsorption patterns, driven by interplay of permanent electrostatic and dispersion effects, and inducing shifting in optical properties, making them excellent candidates for light-harvesting devices.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Jiande Gu, Jing Wang, Jerzy Leszczynski
Summary: The study found three different types of Fe single atom sites on the (110) surface of gamma-alumina, with the tri-coordinated Fe-I position being the most stable. The replacement of Al by Fe results in charge redistributions of neighboring O atoms, and p orbitals of the oxygen atoms on the surface phase contribute significantly to the LUMO in the tri-coordinated Fe-I substitution. This activation of oxygen suggests the presence of an important source of reactive oxygen during Fe catalytic oxidation of CO processes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Metallurgy & Metallurgical Engineering
Yu-xi Lu, Shuai Wang, Zhan-fang Cao, Xin Ma, Hong Zhong
Summary: The relationships between the structure of oxime compounds and their flotation performances were investigated. It was found that introducing different substituents at specific positions in the oxime compounds could enhance certain properties, such as acidity and hydrophobicity, leading to improved flotation efficiency. Additionally, structural optimization resulted in the development of three efficient collectors, demonstrating the effectiveness of structural modification in enhancing the flotation separation performances of oxime compounds.
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
(2022)
Article
Environmental Sciences
Ninghan Wei, Cheng Zhao, Xiaomei Hu, Zhangfa Tong, Junge Yun, Xueying Jiang, Chengxian Liu, Keju Wang, Yun Zou, Zhihang Chen
Summary: The facet-dependent reactivity of Cr\Mn catalysts for NH3-SCR of NOx was investigated using characterizations and density functional theory calculations. The (100) facet of CrMn1.5O4 catalyst exhibited the best low-temperature SCR activity, which was attributed to its increased specific area, electron transfer, concentration of Mn4+ and O alpha, surface acidity, and adsorption/activation capacity for NH3 and NOx. DFT calculations revealed that the (100) facet had the strongest affinity for NH3 and NO due to its unique bonding and abundant charges transfer near the active adsorption sites.
SCIENCE OF THE TOTAL ENVIRONMENT
(2023)
Article
Chemistry, Multidisciplinary
Mitrali Biswas, Sanchaita Dey, Abhishek Das, Tapan Kanti Paine, Sanjib Panda, Goutam Kumar Lahiri
Summary: This study demonstrates the unexplored behavior of redox-active bis(aldimine) congener towards dioxygen activation and subsequent functionalization. The complexes formed were characterized and their redox behavior was analyzed through structure, spectroscopy, and calculations.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Physical
Aili Feng, Yanhong Liu, Yiying Yang, Rongxiu Zhu, Dongju Zhang
Summary: Density functional theory calculations were used to investigate the mechanism and selectivity of the manganese-catalyzed oxidative C(sp(3))-H methylation reaction. The calculations revealed detailed mechanisms for the preactivation of the catalyst, formation of oxidant species, hydroxylation of the substrate, and methylation of the intermediate. The study identified key intermediates and active oxidants, and explained the alpha-site selectivity based on electronic effects.
Article
Chemistry, Physical
Shweta Mehta, Kavita Joshi
Summary: This study investigates the interaction of methanol with different surface structures of zinc oxide (ZnO) using Density Functional Theory (DFT). The results show that the surface structure of ZnO has a significant impact on the adsorption and reaction of methanol.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Razia, Manjusha Chugh, Madhav Ranganathan
Summary: This study introduces a method to calculate the surface energy of clean surfaces by separating the contributions of the pseudo-hydrogen layer, and proposes a modified plane stress condition suitable for slabs with a passivated bottom layer. It is found that the unreconstructed surface exhibits compressive stress, which is relieved through surface reconstructions.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Suresha N. N. Deveshegowda, Ji-Rui Yang, Zhang Xi, Omantheswara Nagaraja, Kashifa Fazl-Ur-Rahman, Bhanuprakash C. C. Narasimhachar, Gautam Sethi, Ganga Periyasamy, Mahendra Madegowda, Shobith Rangappa, Vijay Pandey, Peter E. E. Lobie, Basappa Basappa
Summary: Bioactive dihydropyrimidinones (DHPs) were synthesized via a multicomponent Biginelli reaction catalyzed by nano-zirconium dioxide. The DHPs exhibited a good correlation between the computed and experimental parameters. The ligands 4d and 4e showed inhibition of cell proliferation with IC50 values of 11.8 and 15.8 muM, respectively, and bioinformatic analysis revealed their similarity to rosiglitazone, suggesting their potential as synthetic PPAR-gamma ligands.
Article
Chemistry, Multidisciplinary
Susana Portela, Israel Fernandez
Summary: The potential application of eta(6)-metalated aryl iodides as organocatalysts has been investigated using computational methods. It was found that these species exhibit enhanced halogen bonding donor ability compared to their demetalated counterparts, leading to a significant acceleration of the Diels-Alder cycloaddition reaction. The factors behind this acceleration, as well as the endo-exo selectivity and the influence of the transition metal fragment, were quantitatively explored using the Activation Strain Model and Energy Decomposition Analysis methods.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Physical
Yi Yang, Cheng Liu, Olga A. Syzgantseva, Maria A. Syzgantseva, Shuang Ma, Yong Ding, Molang Cai, Xuepeng Liu, Songyuan Dai, Mohammad Khaja Nazeeruddin
Summary: A new crystallization pathway (RCP) is reported to suppress defects in vertically oriented 2D perovskite films, leading to highly homogeneous and stable films with improved optoelectronic properties. By controlling the adsorption of additives on crystal planes, large grains are encouraged to form, ultimately enhancing the performance of solar cells.
ADVANCED ENERGY MATERIALS
(2021)
Article
Polymer Science
Maria A. Syzgantseva, Olga A. Syzgantseva
Summary: Metal-polymer interactions, specifically between polymethacrylic acid (PMAA) and Ca2+ cation, were studied at an atomistic level to understand the formation of composite materials. The study focused on the coordination patterns of carboxylic groups, impact of PMAA protonation state on polymer cross-linking, and dynamics of Ca cross-linking process in a polymer-rich environment. The findings provide insights into the mechanism of Ca-PMAA hydrogel formation and the structure of metal cross-links, essential for optimizing experimental conditions for polymer composites.
Article
Chemistry, Physical
Albertus Adrian Sutanto, Vellaichamy Joseph, Cansu Igci, Olga A. Syzgantseva, Maria A. Syzgantseva, Vygintas Jankauskas, Kasparas Rakstys, Valentin I. E. Queloz, Ping-Yu Huang, Jen-Shyang Ni, Sachin Kinge, Abdullah M. Asiri, Ming-Chou Chen, Mohammad Khaja Nazeeruddin
Summary: Two structural isomers of carbazole with triarylamine substitution were synthesized and studied for their impact on various properties. One isomer, Car[2,3], exhibited the highest power conversion efficiency in perovskite solar cells, attributed to efficient hole transport due to suitable energy alignment.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Cheng Liu, Cansu Igci, Yi Yang, Olga A. Syzgantseva, Maria A. Syzgantseva, Kasparas Rakstys, Hiroyuki Kanda, Naoyuki Shibayama, Bin Ding, Xianfu Zhang, Vygintas Jankauskas, Yong Ding, Songyuan Dai, Paul J. Dyson, Mohammad Khaja Nazeeruddin
Summary: This study developed a dopant-free D-pi-A type HTM, CI-TTIN-2F, which provides multisite defect-healing effects on CsPbI3 surface, significantly improving the photovoltaic efficiency and thermal stability of CsPbI3 perovskites.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Baohuan Wei, Monica Calatayud
Summary: Titanium oxide (TiO2) is a widely used oxide in various technological and industrial applications. The study focuses on the interaction of hydrogen with TiO2 surface, investigating the diffusion paths from surface to subsurface and the factors influencing this process. The results suggest that surface topology and reduction degree are valid strategies to tune the surface-to-bulk migration process for hydrogen diffusion.
TOPICS IN CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Giulia Mancardi, Matteo Alberghini, Neus Aguilera-Porta, Monica Calatayud, Pietro Asinari, Eliodoro Chiavazzo
Summary: This study investigates the aggregation of titanium dioxide nanoparticles using a multi-scale technique and discovers three new molecular descriptors that can predict the toxicity of materials, enabling safe design strategies.
Article
Energy & Fuels
Cansu Igci, Hiroyuki Kanda, So-Min Yoo, Albertus Adrian Sutanto, Olga A. Syzgantseva, Maria A. Syzgantseva, Vygintas Jankauskas, Kasparas Rakstys, Mounir Mensi, Hobeom Kim, Abdullah M. Asiri, Mohammad Khaja Nazeeruddin
Summary: Three BDP-based organic small molecules, CB-1, CB-2, and CB-3, were synthesized as HTMs for PSCs. Among them, CB-2 exhibited the highest PCE due to its highly planar conformation and defect passivation effect. These properties highlight the great potential of CB-2 as an HTM for efficient and stable PSCs.
Article
Physics, Condensed Matter
Yarkin Aybars Cetin, Benjami Martorell, Francesc Serratosa, Neus Aguilera-Porta, Monica Calatayud
Summary: Titanium dioxide is a crucial material in various fields, but has been banned as a food additive due to toxicity. This study calculates chemical descriptors to understand the surface reactivity of TiO2 and benchmark the descriptors for different computational schemes.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Chemistry, Applied
Etienne P. Hessou, Michael Badawi, Laetitia Valentin, Guy Atohoun, Stanislaw Dzwigaj, Monica Calatayud, Frederik Tielens
Summary: Copper and manganese modified zeolites are important for selective oxidation catalytic reactions. This study combines experimental and theoretical analysis to understand the incorporation of Cu2+ and Mn2+ in the zeolite framework and the nature of active sites.
TOPICS IN CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Gaofeng Chen, Olga A. Syzgantseva, Maria A. Syzgantseva, Shuliang Yang, Guihua Yan, Li Peng, Changyan Cao, Wenxing Chen, Zhiwei Wang, Fengjuan Qin, Tingzhou Lei, Xianhai Zeng, Lu Lin, Weiguo Song, Buxing Han
Summary: By anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix, we designed a diatomic catalyst (Co/Cu-N-C) that exhibits outstanding performance in higher alcohol synthesis. With a CO conversion of 81.7%, it achieves a C(2+)OH selectivity of 58.5% and a remarkable C2+OH STY of 851.8 mg/g center dot h. The N-4-Co-1 and Cu-1-N-4 sites demonstrate excellent synergistic effects, with CO adsorbing on the Co site and surrounding nitrogen sites acting as a hydrogen reservoir for CO reduction reactions to form CHxCo. Simultaneously, the Cu sites stabilize a CHOCu species to interact with CHxCo, promoting barrier-free formation of C-2 species and enhancing the selectivity of higher alcohols.
Article
Chemistry, Physical
Tianwei Xue, Olga A. Syzgantseva, Li Peng, Maria A. Syzgantseva, Ruiqing Li, Guangkuo Xu, Daniel T. Sun, Rongxing Qiu, Chengbin Liu, Shu Zhang, Tiezhu Su, Peifeng Su, Shuliang Yang, Jun Li, Buxing Han
Summary: In this work, a robust imine-linked 2D COF was synthesized in supercritical CO2, which could maintain a high surface area and prevent pore collapse after vacuum activation. The method used in this study is universal and has the potential to be applied in the synthesis of other imine-linked 2D COFs.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Xavier Deraet, Jan Turek, Mercedes Alonso, Frederik Tielens, Bert M. M. Weckhuysen, Monica Calatayud, Frank De Proft
Summary: This paper investigates the adsorption behavior of single late transition metals on a defect-free anatase surface using periodic density functional theory calculations. The results reveal that the interaction strength between the transition metals and the support can be attributed to electron transfer, s-d orbital hybridization effects, or a synergistic effect between both factors. Palladium shows deviating adsorption behavior, which is likely associated with the lower dissociation enthalpy of the Pd-O bond. The reactivity of these systems is evaluated using the Fermi weighted density of states approach, and a model is proposed to predict the adsorption strength of CO on anatase-supported d-metal atoms.
Article
Chemistry, Multidisciplinary
Beata Taudul, Frederik Tielens, Monica Calatayud
Summary: In this study, a computational protocol is developed to accurately calculate the Raman response of pure TiO2 materials. The origin of the Raman peaks is analyzed, and a structure-Raman mapping is performed to account for various factors. This study provides guidelines for accurate characterization of different titania systems using Raman spectroscopy.
Article
Materials Science, Multidisciplinary
Rita Maji, Elena Degoli, Monica Calatayud, Valerie Veniard, Eleonora Luppi
Summary: Currently, the most accurate method to describe excitons in solids is GW-BSE, but the computation cost has led to the alternative use of TDDFT. Long-range corrected exchange-correlation kernels and range-separated hybrid functionals are the most efficient strategies to describe optical spectra in TDDFT. This study compares their performance for describing excitons in solids and provides new perspectives for theoretical developments of these functionals.
Correction
Chemistry, Physical
Sanghyun Paek, Sher Bahadar Khan, Marius Franckevicius, Rokas Gegevicius, Olga A. Syzgantseva, Maria A. Syzgantseva, Sachin Kinge, Abdullah M. Asiri, Cristina Roldan-Carmona, Mohammed Khaja Nazeeruddin
JOURNAL OF MATERIALS CHEMISTRY A
(2021)