Article
Chemistry, Multidisciplinary
Mohammadjavad Karimi, Elham S. Tabei, Remi Fayad, Mohamed R. Saber, Evgeny O. Danilov, Cameron Jones, Felix N. Castellano, Francois P. Gabbai
Summary: The study found that both isomeric complexes cleanly converted into the platinum germyl complex in the presence of a chlorine trap, with high quantum yields. The conversion of the Ge-IV-Pt-II isomer into the platinum germyl complex is a rare example of a light-induced transition-metal/main-group-element bond-forming process. Transient-absorption-spectroscopy studies on the Ge-III-Pt-III isomer suggest a ligand arene-Cl- charge-transfer complex as an intermediate.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Yumiao Dong, Qinhui Xie, Shuo Wu, Junbo Li, Lei Sun, Wei Ji
Summary: The adsorption mechanism of 4-MBA on TiO2 surfaces is found to be highly dependent on the exposure of acid sites, with preferential adsorption on Bronsted acid sites of a-TiO2 through a carboxyl group and on Lewis acid sites of c-TiO2 through a sulfhydryl group. Furthermore, 4-MBA molecules may form multilayer adsorption on TiO2 surfaces through hydrogen bonding and/or pi-pi stacking interactions. These findings provide new insights into the chemical enhancement mechanism for TiO2-4-MBA systems and offer theoretical guidance for the modification of TiO2 surfaces with organic molecules containing carboxyl and sulfhydryl groups.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jakub Kocak, Eli Kraisler, Axel Schild
Summary: When a molecule dissociates, the Kohn-Sham (KS) and Pauli potentials form step structures, critical for describing dissociation and charge-transfer processes. The exact electron factorization (EEF) provides an explanation for these steps, showing they are a result of spatial electron entanglement and charge transfer. Additionally, two methods to reproduce the potentials during dissociation are proposed, offering insights into the encoding of many-electron effects in a one-electron theory.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Xuli Li, Shaojia Song, Yangqin Gao, Lei Ge, Weiyu Song, Tianyi Ma, Jian Liu
Summary: A noble-metal free photocatalytic system of NC@Co-NCT/CdS was fabricated to enhance water splitting for H-2 production. The optimal photocatalytic activity of NC@Co-NCT/CdS was found to be 3.8 mmol h(-1) g(-1), approximately 5.8 times that of CdS. This study reveals a novel photoelectron transfer channel in the heterojunction interfaces, facilitating the migration and separation of photo-induced charge carriers of CdS, and suggests that Co nanoclusters can act as active sites to boost the H-2 evolution reaction.
Article
Chemistry, Multidisciplinary
Atanu Jana, Masatoshi Ishida, Hiroyuki Furuta
Summary: The newly synthesized BTTF7-F and BTTF8 exhibit intrinsic intramolecular charge transfer properties and the control of intra-CT process can be achieved by incrementally adding TTF units to the macrocyclic core.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Sirui Yang, Chen Cao, Amjad Islam, Shanshan Sun, Ziqi Deng, Jiayu Li, Shaofei Ni, Qing-Xiao Tong, Ming-De Li
Summary: Two deep-blue luminescent materials were designed using the bipolarity of 1,2-diphenylphenanthroimidazole, with investigation of their excited-state evolution and interchromophoric interactions revealing factors such as electronic nature, structure, and solvent polarity influencing intramolecular charge transfer lifetime.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Donghyeon Kang, Hyeon Yeong Lee, Joon-Ha Hwang, Sera Jeon, Dabin Kim, SeongMin Kim, Sang-Woo Kim
Summary: This study investigated the impact of molecular structure deformation on the triboelectric properties of PTFE induced by contact force using density functional theory (DFT). The results showed that deformation enhanced the negative triboelectric property of PTFE mainly due to the electron-deficient state of carbon atoms leading to enhanced local dipole.
Article
Chemistry, Physical
Costanza Ronchi, Federico A. Soria, Lorenzo Ferraro, Silvana Botti, Cristiana Di Valentin
Summary: By using time-dependent density functional theory calculations, this study investigates the absorption properties of two catechol-like molecules anchored to spherical anatase TiO2 nanoparticles. The research reveals a direct charge transfer injection mechanism and the impact of molecular benzene ring orientation on absorption intensity.
MATERIALS TODAY ENERGY
(2021)
Article
Physics, Applied
Andrew C. Antony, Dean Thelen, Nikolay Zhelev, Kaveh Adib, Robert G. Manley
Summary: The study reveals that contact charging between metals and hydroxylated SiO2 induces electronic states at the SiO2 surface, with the magnitude of these states varying with the type of metal and the density of surface defect states.
JOURNAL OF APPLIED PHYSICS
(2021)
Article
Chemistry, Physical
Aysenur Gencer, Sezgin Aydin, Ozge Surucu, Xiaotian Wang, Engin Deligoz, Gokhan Surucu
Summary: In this study, the hydrogen storage properties of Li-decorated Hf2CF2 MXene layer were investigated using first-principles calculations. The results show that the Li-decorated layer exhibits stable and convenient adsorption characteristics, making it a promising candidate for hydrogen storage applications.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Environmental
Qian Zhang, Die Guo, Yan-ling Yang, Jun-ming Hong
Summary: To improve the electrocatalytic performance, 2D/2D MXene/RGO heterostructures were prepared by constructing a Ti-O-C connection. The Ti-O-C connection facilitates charge transfer and creates active sites for active species generation. Active species, such as O2 ·-, 1O2, and active chlorine, were identified as responsible for the excellent catalytic activity of MXene/RGO. Charge transfer and Ti-OH edges play critical roles in active chlorine generation. This study provides a mechanism discussion for improving electrocatalytic performance over stable MXene/RGO heterostructures.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
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
Spectroscopy
Hongbin Zhan, Hengwei Zhang, Yi Wang, Yaping Tao, Jing Tian, Xu Fei
Summary: This study investigated the fluorescence mechanism of HN-ClO and HN-ClO-F probes using DFT and TDDFT, showing distinct charge distribution and fluorescence characteristics in their excited states. The strong fluorescence of HN-ClO-F is attributed to the planar structure-induced charge coupling, while the weak fluorescence of HN-ClO is caused by inter-system crossing.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2022)
Article
Chemistry, Physical
Valerio Giuso, Elise Jouaiti, Cristina Cebrian, Sabrina Parant-Aury, Nathalie Kyritsakas, Christophe Gourlaouen, Matteo Mauro
Summary: This study presents a series of four cationic Zn-II complexes (Zn1-Zn4) coordinated by substituted bis-imidazo[1,2-a]pyridine (ImPy) ligands (L1-L4). These complexes exhibit intense emission in the near-UV to blue range with high photoluminescence quantum yields in DMF solution. Moreover, complex Zn4 shows solvatochromic behavior and a unique structureless green photoluminescence in the solid state.
Article
Chemistry, Physical
Ambrish Kumar Srivastava
Summary: The study shows that C-60 fullerene can be activated by the surface interaction with superalkali clusters, forming SAC(60) complexes with enhanced dipole moment and energy gap. This is in contrast to endohedral SA@C-60 complexes, which have negligible dipole moment and lower energy gap.
Article
Chemistry, Physical
Erhao Gao, Wenjing Feng, Qi Jin, Li Han, Yi He
Summary: The influence of K-doping on the reactive oxygen species and elementary reactions of HCHO catalytic oxidation was investigated using density functional theory (DFT). The introduction of K-doping changed the electronic structures of Ce and O, facilitating the adsorption and activation of HCHO and O2 molecules, enhancing lattice oxygen mobility, and reducing the energy barrier for HCHO oxidation. K-doping also promoted the formation of hydroxyl groups, facilitating HCHO adsorption and oxidation.
Article
Chemistry, Physical
Hao Fu, Zhangliang Xu
Summary: In this study, the adsorption mechanisms and detection performance of formaldehyde, ammonia, and sulfur dioxide on undoped and metal-doped ZnO surfaces were investigated using density functional theory. The results showed that formaldehyde and ammonia were physically adsorbed on the undoped ZnO surface, while sulfur dioxide was weakly chemisorbed. The adsorption energy was enhanced when ZnO was doped with metals. These findings provide theoretical guidance for the application of ZnO substrate materials in gas sensitivity research.
Article
Chemistry, Physical
Atsushi Nomura, Tohru Kurosawa, Migaku Oda, Satoshi Demura, Shogo Kuwahara, Sora Kobayashi, Hideaki Sakata
Summary: The study investigates the tunneling spectra of 1T-TiSe2 in the CDW state and the dip structure below the Fermi level, aiming to determine whether this dip is a CDW gap. The answer to this question is crucial for understanding the driving mechanism of CDW.
Article
Chemistry, Physical
A. S. Petrov, D. I. Rogilo, A. I. Vergules, V. G. Mansurov, D. V. Sheglov, A. V. Latyshev
Summary: This study investigates Si mass transport and morphological transformations on the Si(111) surface during (root 3 x root 3)-Sn reconstruction formation and Si homoepitaxy. The research shows that the formation of different Sn phases at different temperatures affects the Si island nucleation and monatomic step shift, which in turn impact the morphology of the Sn/Si(111) interface. Electromigration-induced drift of disordered Sn domains leads to enhanced noncompensated Si mass transport and surface roughening.
Article
Chemistry, Physical
D. V. Gruznev, L. V. Bondarenko, A. Y. Tupchaya, A. A. Yakovlev, A. N. Mihalyuk, A. V. Zotov, A. A. Saranin
Summary: Deposition of thallium (Tl) onto the Au/Si(111)5 x 2 reconstruction followed by annealing results in the formation of a surface structure with 4 x 2 periodicity. The immiscibility of Au and Tl leads to the migration of Tl atoms over the Si chains. Thallium donates electrons to the surface, converting the metallic surface into an insulating state and altering the inter-chain distance within the array of Au atomic wires.
Article
Chemistry, Physical
Simone Giusepponi, Francesco Buonocore, Barbara Ferrucci, Massimo Celino
Summary: Using ab-initio calculations, the interaction between lead adatom and both clean and doped iron (100) surfaces was investigated. It was found that the lead adatom prefers to adsorb in the hollow site, which is more stable compared to the top and bridge sites, and in this position, it is energetically favorable over the iron adatom. Moreover, lead adsorbed in the hollow site of the iron (100) surface doped with chromium was found to create a more stable system compared to nickel-doped surfaces with an iron adatom in the same position. The study also explored inter-layer distances, bonding mechanisms, magnetic behaviors, and charge density differences. The results provide insights into the role of doping in the interaction between lead adatom and iron surface, and have implications for the analysis of corrosion processes caused by liquid lead.
Article
Chemistry, Physical
Shuo Zhang, Jin-Ho Choi
Summary: The recent synthesis of two-dimensional layered WSi2N4 has attracted attention due to its potential applications. This study investigates the catalytic performance of WSi2N4 monolayers with nitrogen vacancies in the hydrogen evolution reaction using first-principles calculations. The results show that the defective WSi2N4 monolayers exhibit remarkably high catalytic activity comparable to platinum catalysts. Electronic structure calculations also reveal the emergence of spin-polarized states due to the introduction of nitrogen vacancies.
Article
Chemistry, Physical
Xiaoyan Yu, Xin Cao, Wei Kang, Shanhua Chen, Ao Jiang, Yuhao Luo, Wenwei Deng
Summary: First-principles calculations were used to investigate the electronic properties of a TiO2 heterostructure modified with Bi2Te3 co-catalyst. The study revealed that the Bi2Te3/TiO2 interface introduced optimal band offsets, effectively suppressing electron-hole recombination and enhancing the utilization efficiency of photo-generated carriers. Additionally, the Bi2Te3 co-catalyst introduced extra catalytic active sites, further boosting the photo-catalytic hydrogen evolution efficiency.
Article
Chemistry, Physical
Filippo Longo, Emanuel Billeter, Selim Kazaz, Alessia Cesarini, Marin Nikolic, Aarati Chacko, Patrik Schmutz, Zbynek Novotny, Andreas Borgschulte
Summary: Alkaline water electrolysis is a simple and efficient method for renewable hydrogen production, utilizing cheap and abundant transition metals. The catalytic properties of Ni materials are enhanced by the formation of oxidized compounds on the surface. The high electrocatalytic activity of Ni (oxy)-hydroxides is directly related to water intercalation in the passivation layer, supporting the hypothesis of a water mediated OH- diffusion mechanism. The self-organization of the surface structure during passivation layer formation enables high electrode performance.
Article
Chemistry, Physical
Mohan Kumar Kuntumalla, Miriam Fischer, Alon Hoffman
Summary: By investigating the bonding, retention, and thermal stability of nitrogen in H-Diamond (100), it was found that nitrogen can partially recover its bonding with carbon atoms after high-temperature annealing, indicating a high thermal stability of nitrogen in diamond.
Article
Chemistry, Physical
Dong Yue, Liangying Wen, Rong Chen, Jianxin Wang, Zhongqing Yang
Summary: The adsorption behavior of Cl2 molecules on the TiC surface and the formation and transfer of reaction products were studied using first-principles ab initio calculations. The results show that the Cl atoms bonded to the surface Ti atoms are more stable, and the TiCl3 intermediate is easier to form than the TiCl2 intermediate.
Article
Chemistry, Physical
Yatao Wang, Peng Zhang, Hongjuan Li, Qiuju Xu, Shujun Liu, Xiaopeng Liu, Xuehua Guo, Yitao Li, Jinzhang Liu, Sen Dong, Zhi Wei Seh, Qianfan Zhang
Summary: In this study, the adsorption performance of two types of metal-organic frameworks (MOFs) for thiophene and benzene was experimentally investigated. The results showed that IZE-1 exhibited high selectivity and superior adsorption capacity for thiophene, especially at low concentrations. First-principles calculations and molecular dynamics simulations provided insights into the mechanism of thiophene adsorption and the high selectivity observed. This research demonstrates the potential of MOFs for thiophene adsorption, particularly at high concentrations.
