Article
Biochemical Research Methods
Na Lv, Xiangyu Guo, Lihong Zhang, Irfan Ali Soomro, Shiping Huang
Summary: In this study, the geometries, electronic properties, and chemical bonding of (VH2)n (n =10-30) nanoclusters were systematically investigated using a combination of artificial bee colony optimization with density functional theory calculations. The results indicate that the coordination numbers of V-H fluctuate significantly in the nanoclusters, and there is a large overlap between the d orbitals of V atoms and the s orbitals of H atoms, forming sigma bonds.
JOURNAL OF MOLECULAR GRAPHICS & MODELLING
(2021)
Article
Chemistry, Organic
Wenting Wang, Lin Zhao, Hui Wu, Youqing He, Ge Wu
Summary: A metal-free oxidative trideuteromethylthiolation of alkenes using CD3SSO3Na as an oxidant has been developed. The aminotrideuteromethylthiolation of a three-component reaction could be easily achieved in the presence of a cobalt catalyst. The divergent trideuteromethylthiolation of alkenes, readily available trideuteromethylthiolation reagent, and versatile synthetic strategy enable late-stage modification of drug molecules.
Article
Chemistry, Multidisciplinary
Raagya Arora, Umesh Waghmare, C. N. R. Rao
Summary: This study investigates various 2D lattices of Group IV chalcogenides to understand the nature of metavalent bonding (MVB). It is found that honeycomb lattices adhere to the 8-N rule and exhibit covalent bonding, while square and orthorhombic structures display in-plane MVB driven by p-p orbital interactions, with cationic lone pairs inducing out-of-plane puckering.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Analytical
Nathaniel L. Dominique, Shelby L. Strausser, Jacob E. Olson, William C. Boggess, David M. Jenkins, Jon P. Camden
Summary: This study investigates the stability and potential biological applications of N-heterocyclic carbene (NHC) self-assembled monolayers (SAMs) on gold surfaces, while utilizing laser desorption ionization mass spectrometry (LDI-MS) to explore the surface chemistry of NHC. By studying NHC-functionalized gold nanoparticles using LDI-MS, insights into the packing of NHC monolayers on gold surfaces and the stability of NHC ligands post-ligation were gained. The ability of LDI-MS to probe postsynthetic modifications of anchored NHCs, such as the reduction of nitro-NHC-AuNPs to amine-NHC-AuNPs, highlights its importance for current and future applications of NHC surfaces.
ANALYTICAL CHEMISTRY
(2021)
Article
Multidisciplinary Sciences
Yuanhui Sun, Lei Zhao, Chris J. Pickard, Russell J. Hemley, Yonghao Zheng, Maosheng Miao
Summary: Most metals have simple structures, but undergo complex transitions on compression. First-principles calculations can reproduce observed structures and transitions, but a unified predictive theory is lacking. By analyzing electronic properties, a simple theory shows that the stability of metal structures is governed by electrons in interstitial orbitals and their chemical interactions. This theory provides a basis for understanding and predicting structures in solid compounds and alloys.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Physical
Sheng-Jie Lu
Summary: This study investigates the geometric structures of platinum-silicon clusters, revealing different geometries and most stable configurations in various ionic states. Interestingly, some platinum-silicon clusters exhibit sigma plus pi double bonding characters.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Zhijie Yang, Linqin Mu, Dong Hou, Muhammad Mominur Rahman, Zhengrui Xu, Jue Liu, Dennis Nordlund, Cheng-Jun Sun, Xianghui Xiao, Feng Lin
Summary: This study investigates dopant distribution, phase propagation, and local chemical changes in multi-element-doped LiNiO2 materials using spectroscopic, imaging, and scattering techniques. Results show dynamic redistribution of dopants in the Ni(OH)(2) lattice during early stage calcination, allowing for targeted doping control. Ni oxidation exhibits depth-dependent characteristics, with heterogeneous phase propagation in the early stage of calcination.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Farid Kameche, Wajdi Heni, Siham Telitel, Loic Vidal, Sylvie Marguet, Ludovic Douillard, Celine Fiorini-Debuisschert, Renaud Bachelot, Olivier Soppera
Summary: The localized surface plasmon-induced photopolymerization of free-radical acrylate monomers is an efficient method for preparing metal/polymer hybrid nanoparticles with precise control over the thickness and distribution of the polymer on the nanoparticle surface. Experimental studies have shown that the photochemical pathway may be the main mechanism, although various mechanisms involving electromagnetic hot spots, thermoplasmonic effects, and electrochemical processes have been proposed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Materials Science, Multidisciplinary
Miguel Betancourt-Ponce, Christian Morales-Guzman, Perla Cruz-Tato, Eduardo Nicolau
Summary: Forward osmosis (FO) is a passive liquid separation process that has the potential to produce clean water with minimal energy consumption. By studying the effects of TMAO analogues on PSf membranes, it was found that these additives significantly influence membrane formation and properties.
ACS APPLIED POLYMER MATERIALS
(2022)
Article
Materials Science, Multidisciplinary
Miguel Betancourt-Ponce, Christian Morales-Guzman, Perla Cruz-Tato, Eduardo Nicolau
Summary: FO is a passive liquid separation process that has the potential to produce clean water with minimal energy consumption. To achieve this potential, membranes with enhanced properties, such as high fouling resistance and solute rejection, must be developed.
ACS APPLIED POLYMER MATERIALS
(2022)
Article
Energy & Fuels
Leilei Xu, Yachao Chang, Mark Treacy, Yuchen Zhou, Ming Jia, Xue-Song Bai
Summary: This study proposes a simplified chemical kinetic mechanism for ammonia/n-heptane blend fuels and further optimizes the mechanism using an optimization algorithm. The mechanism is validated against experimental data and shows accurate predictions of combustion processes under a wide range of conditions, with high computational efficiency.
Article
Chemistry, Multidisciplinary
Ruo-Ya Wang, Jing-Xuan Zhang, Xue-Lian Jiang, Nana Ma, Xuenian Chen, Cong-Qiao Xu, Jun Li
Summary: Borane clusters and their derivatives have been extensively studied in inorganic chemistry for their intriguing multi-center bonding patterns and physicochemical properties. Through systematic theoretical investigation, this study reveals that the electronic structure and stability of these clusters can be modulated by the size of the boron cage and electronegativity of the ligand, with fragment orbital energy matching and orbital overlap playing crucial roles in the covalency of the cluster. Additionally, the ionic electrostatic interaction decreases as the ligand becomes heavier, while multi-center bonding covalency determined by the orbital interaction increases, contributing to the sigma aromaticity and superb stability of the clusters.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Fangying Zhang, Wangwang Fang, Fanyong Yan, Bowei Wang, Dan Zhang, Tao Wang, Guoyi Bai, Ligong Chen, Yang Li, Xilong Yan
Summary: CeO2-promoted Co-N-C hybrids were prepared using the strategy of solid solution construction and exhibited satisfactory performance and stability in catalytic reactions, with improved resistance to sulfur poisoning.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Dakota M. Merriles, Anthony London, Erick Tieu, Christopher Nielson, Michael D. Morse
Summary: Resonant two-photon ionization experiments were conducted to measure the bond dissociation energy (BDE) of lanthanide-carbon bonds. Quantum chemical calculations were used to investigate the electronic structure of these compounds. Despite having similar ground electronic configurations, LaC, CeC, PrC, and NdC exhibit a peculiar range of 1.30 eV in their BDEs.
INORGANIC CHEMISTRY
(2023)
Review
Geochemistry & Geophysics
Frank K. Crundwell
Summary: This paper presents a novel surface-vacancy model for dissolution processes, which envisions ions departing from the surface separately and leaving behind an excess surface charge, affecting the rate of departure and reaction progress. The model can explain orders of reaction, equilibrium conditions, acceleration or deceleration of rates, and the effect of impurities, while also predicting phenomena like 'partial equilibrium' not considered by other models. The underlying physical model has implications beyond dissolution studies and can be independently verified through measurements of surface charge.
Article
Biochemistry & Molecular Biology
Vlasta Bonacic-Koutecky, Xavier Le Guevel, Rodolphe Antoine
Summary: Luminescent gold nanoclusters have attracted attention as efficient theranostic targets for imaging and therapeutics due to their easy synthesis, tunable optical properties, and tumor targeting, making them potential candidates for sensitive diagnosis and effective therapeutic applications, especially in the field of oncology.
Article
Chemistry, Multidisciplinary
Peng-Fei Han, Ying-Jin Wang, Qiang Sun, Hua-Jin Zhai
Summary: Combining quantum chemical calculations with unbiased global searches, a unique binary B7Mg4+ cluster has been revealed, in which a vertically oriented Mg-2 dimer is incorporated into a ringent B-7 disk, forming a hybrid Mg2B7 molecular wheel with pseudo-seven-fold in-plane coordination. The concept of electronic transmutation has been used to elucidate the unique plier shape of the cluster.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Ying-Jin Wang, Lin-Yan Feng, Miao Yan, Hua-Jin Zhai
Summary: The beryllium-doped Be3B11- cluster has two nearly isoenergetic isomers with different geometries. The structural transformation of the boron skeleton is enabled by the electrostatic interaction between beryllium atoms and the boron skeleton. This cluster exhibits dynamic fluxionality and spherical aromaticity due to the free migration of boron atoms and the presence of delocalized pi bonds.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Rong-Xin Yue, Shu-Juan Gao, Peng-Fei Han, Hua-Jin Zhai
Summary: Despite the isovalency between Al and B elements, Al-doping in boron clusters can lead to a unique sandwich di-Al-doped boron cluster, Al2B8. This cluster exhibits dynamic fluxionality with a vertically sliding or rotating Al-2 rod on a B-8 plate, despite no direct Al-Al interaction. The cluster shows charge-transfer complex behavior and has a magic 6 pi/6 sigma double aromaticity.
Editorial Material
Chemistry, Physical
Michele Ceriotti, Lasse Jensen, David E. Manolopoulos, Todd Martinez, David R. Reichman, Francesco Sciortino, C. David Sherrill, Qiang Shi, Carlos Vega, Lai-Sheng Wang, Emily A. Weiss, Xiaoyang Zhu, Jenny Stein, Tianquan Lian
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Rui Sun, Caixia Yuan, Hua-Jin Zhai, Yan-Bo Wu
Summary: In this work, we computationally designed a series of aluminum chalcogenide clusters NAl4X4+ (X = S, Se, Te) with a desired planar tetracoordinate nitrogen and significantly improved chemical stability. These clusters are stabilized by peripheral chalcogen atoms and electron-compensated aluminum atoms via X ? Al p back bonds.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
G. Stephen Kocheril, Han-Wen Gao, Lai-Sheng Wang
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Anton S. Pozdeev, Wei-Jia Chen, Hyun Wook Choi, Maksim Kulichenko, Dao-Fu Yuan, Alexander I. Boldyrev, Lai-Sheng Wang
Summary: Copper is capable of mediating the formation of bilayer borophenes. Copper-boron binary clusters are used to investigate the interactions between copper and boron, which are crucial for understanding the growth mechanisms of borophenes on copper substrates. In this study, joint photoelectron spectroscopy and theoretical calculations were conducted on two di-copper-doped boron clusters, Cu2B3 (-) and Cu2B4 (-). Well-resolved photoelectron spectra were obtained, revealing the presence of low-lying isomers in both cases. Theoretical calculations showed that the global minimum structures of Cu2B3 (-) and Cu2B4 (-) have different arrangements of copper and boron atoms.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Dao-Fu Yuan, Yuan Liu, Yue-Rou Zhang, Lai-Sheng Wang
Summary: The first observation of a polarization-assisted dipole-bound state (DBS) for a molecule with a dipole moment below 2.5 debye is reported. Photoelectron and photodetachment spectroscopies are conducted and a DBS is found only 6 cm-1 below the detachment threshold along with sharp vibrational Feshbach resonances. The observed DBS has pi-symmetry stabilized by the strong anisotropic polarizability of indolyl.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
G. Stephen Kocheril, Han-Wen Gao, Lai-Sheng Wang
Summary: We conducted a temperature-controlled photoelectron imaging study on SbO2-, which was produced from a laser vaporisation source and cooled in a cryogenic 3D Paul trap. We obtained vibrationally resolved photoelectron spectra for the ground state detachment transition and determined the bending frequencies for both SbO2 and SbO2-. Franck-Condon simulations allowed us to estimate the vibrational temperature of the trapped SbO2- anion. We also obtained a near-threshold spectrum of SbO2- at a photon energy of 3.4958 eV, revealing partially resolved rotational structure and providing an accurate measurement of the electron affinity of SbO2.
Article
Biochemistry & Molecular Biology
Peng-Fei Han, Ying-Jin Wang, Lin-Yan Feng, Shu-Juan Gao, Qiang Sun, Hua-Jin Zhai
Summary: Doping alkali metals into boron clusters can compensate for boron's electron deficiency and lead to interesting boron-based binary clusters. We report on the computational design of a three-layered sandwich cluster, Na5B7, which exhibits charge-transfer complex and three-fold aromaticity. Molecular dynamics simulation shows that the sandwich cluster is dynamically fluxional even at room temperature. The Na5B7 cluster offers a new example for dynamic structural fluxionality in molecular systems.
Article
Biochemistry & Molecular Biology
Peng-Fei Han, Qiang Sun, Hua-Jin Zhai
Summary: We predict a new example of boron-based inverse sandwich alloy clusters, V2B7-, through computational global-minimum structure searches and quantum chemical calculations. Chemical bonding analysis reveals that the inverse sandwich cluster is governed by globally delocalized 6p and 6s frameworks, following the (4n + 2) Huckel rule. The skeleton B-B s bonding is shown to be quasi-Lewis-type, roof-like 4c-2e V-B-2-V s bonds, covering the whole surface of the inverse sandwich cluster in a truly three-dimensional manner.
Article
Chemistry, Multidisciplinary
Yue-Rou Zhang, Dao-Fu Yuan, Chen-Hui Qian, Guo-Zhu Zhu, Lai-Sheng Wang
Summary: Although the influence of molecular polarizability on the formation of dipole-bound states (DBSs) is not well understood, this study investigates the role of polarization interactions in the formation of DBSs using carbazolide as a model compound. The study utilizes cryogenic photodetachment spectroscopy and high-resolution photoelectron spectroscopy and reveals the presence of a polarization-assisted DBS, despite the carbazolyl neutral core having a dipole moment smaller than the critical value. The study also provides valuable information about the vibrational modes and electronic states of carbazolide.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Anton S. Pozdeev, Wei-Jia Chen, Maksim Kulichenko, Hyun Wook Choi, Alexander I. Boldyrev, Lai-Sheng Wang
Summary: Researchers have discovered that copper-boron binary clusters have unique covalent bonding structures, which are determined by the high stability of the appropriate-sized boron chain structures in this range. In larger boron chain structures, it is expected that ionic bonding between copper and boron will occur.
SOLID STATE SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Margarita Buzancic Milosavljevic, Antonija Mravak, Martina Peric Bakulic, Vlasta Bonacic-Koutecky
Summary: In this study, the structural, optical, and photovoltaic properties of novel bio-nano hybrids (dye-nanocluster), along with a TiO2 surface model, are investigated for their application in dye-sensitized solar cells (DSSC). Specifically, a group of anthocyanidin dyes covalently bound to silver nanoclusters (NCs) with even or odd number of valence electrons were studied. The results show that the nanoclusters with an even number of valence electrons exhibit better acceptor properties in the hybrids. Additionally, the interaction between the bio-nano (dye-NC) hybrid and the TiO2 surface model was studied in terms of near-infrared absorption and charge separation. Overall, this theoretical study provides insights for the design of novel DSSCs based on bio-nano hybrids at the TiO2 surface.