Article
Chemistry, Inorganic & Nuclear
A. A. Rybakov, S. Todorova, D. N. Trubnikov, A. Larin
Summary: The study evaluated the importance of heterogeneity of a Pd monolayer induced by interaction with a semi-ionic support in catalysis, finding that the hybrid Pd(100)/(111) layer exhibits lower activation barriers and greater stability, suitable for methane dissociation and water-gas shift reaction. Additionally, the characteristics of chemisorption and exothermic reactions on monolayer structures depend on Pd atomic charges and can explain the maximum reaction rate observed at different Pd coverages.
DALTON TRANSACTIONS
(2021)
Article
Nanoscience & Nanotechnology
Jing Zhang, Jiren Wang, Chunhua Zhang, Zongxiang Li, Bing Lu, Jinchao Zhu
Summary: The study found that in the low-pressure zone, lignite and anthracite have a strong adsorption capacity for C2H4, which gradually weakens with increasing pressure; C2H4 and CO2 have similar and concentrated adsorption sites, while O2 and N2 have more adsorption sites and larger adsorption capacities.
Article
Thermodynamics
Han Sun, Akira Kawasaki, Ken Matsuoka, Jiro Kasahara
Summary: Through experimental study on detonation diffraction, we found that the reflection point distance can serve as a new characteristic length, and the critical condition can be expressed using it; the results show that the reflection point distance and critical condition are not affected by channel width, fuel species, or equivalence ratio.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2021)
Article
Engineering, Chemical
Hua Shuai, Junhui Liu, Yesong Teng, Xing Liu, Lingmin Wang, Hanting Xiong, Pengxiang Wang, Jingwen Chen, Shixia Chen, Zhenyu Zhou, Shuguang Deng, Jun Wang
Summary: A pillar-layered metal-organic framework, Ni(sdba)(dabco)0.5, is reported for the one-step production of high-purity ethylene with outstanding selectivity towards ethane and acetylene.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Physical
Ngo Thi Lan, Nguyen Thi Mai, Duong Duc La, Son Tung Ngo, Nguyen Minh Tam, Nguyen Van Dang, Nguyen Thanh Tung
Summary: In this study, the interaction between hydrogen molecules and Au9M2+ clusters was investigated using density-functional theory (DFT). The preferred adsorption configuration of hydrogen on these clusters was found to be influenced by factors such as surface/encapsulated position, relative electronegativity, and coordination number of atoms. The research provides insights into the mechanisms underlying hydrogen adsorption and can aid further theoretical and experimental studies of hydrogenation in nanostructured materials.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Mugdha Ambast, Abhay Gupta, Bhuiyan Md Mushfikur Rahman, Lars C. Grabow, Michael P. Harold
Summary: A transient monolith model is proposed to study NO uptake and release over Pd/SSZ-13, with or without reductants CO or C2H4. Kinetic parameters are estimated using a combination of DFT and experimental data fitting, which helps interpret data features and optimize operating conditions. The model shows higher NO uptake on Pd/SSZ-13 compared to Pd/ZSM-5.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Hui Li, Denghui Wang, Shien Hui
Summary: According to the DFT calculations, NO was more prone to adsorb on the four-coordinated Mn(IV) sites on the MnO2(1 1 0) surface, while O-2 could only stably adsorb in vacancies between adjacent Mn(IV) ions.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Chemical
Ruihan Wang, Qiang Gao, Yeshuang Zhong, Xin Wang, Dingguo Xu
Summary: This study investigated the influence of oxygen (O2) on the C2H6/C2H4 selectivity of a Cr-BTC MOF using density functional theory calculations and grand canonical Monte Carlo simulations. The results showed that O2 formed a superoxo site by antiferromagnetic coupling to the open Cr site, decreasing the dipole moment of the open metal site. The presence of the superoxo site blocked the interaction between Cr and C2H4, altering the gas selectivity.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Engineering, Environmental
Pengbo Hu, Qiyu Weng, Duanle Li, Tao Lv, Shujuan Wang, Yuqun Zhuo
Summary: This study theoretically investigated the effects of flue gas constituents on As2O3 adsorption on γ-Al2O3 surface using DFT, finding that O2 converts most physisorption structures to chemisorption structures and the differences in stable adsorption structures of O2, H2O, SO2, and CO2 are the main factors affecting the positions and quantities of As2O3 physisorption structures. This research provides valuable information for enhancing the capture capacities of γ-Al2O3 in actual flue gas environments.
JOURNAL OF HAZARDOUS MATERIALS
(2021)
Article
Chemistry, Physical
Qiuying Du, Lulu Huang, Jiaqi Fu, Yongjun Cao, Xiaopeng Xing, Jijun Zhao
Summary: Single atom alloy AgCu catalysts, with narrow free-atom-like Cu 3d states in the electronic structure, have attracted much attention for their potential in reducing activation energies and improving catalytic performance. However, the geometric tuning effect of single Cu atoms in Ag catalysts and the structure-activity relationship of AgCu catalysts still need to be explored.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Zhengyi Di, Caiping Liu, Jiandong Pang, Shuixiang Zou, Zhenyu Ji, Falu Hu, Cheng Chen, Daqiang Yuan, Maochun Hong, Mingyan Wu
Summary: This study presents a highly stable metal-organic framework with a unique pore structure for the one-step separation of high-purity ethylene from ethylene and ethane mixtures.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Richard C. Knighton, Lohona K. Soro, Laura Frances-Soriano, Aurora Rodriguez-Rodriguez, Guillaume Pilet, Marc Lenertz, Carlos Platas-Iglesias, Niko Hildebrandt, Loic J. Charbonniere
Summary: Upconversion materials have led to breakthrough applications in solar energy conversion, imaging, and biomedicine. Surprisingly, the best UC performances were obtained for Yb/Tb ratios close to parity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Musen Zhou, Jianzhong Wu
Summary: Efficient separation of C2H4/C2H6 mixtures is important in the petrochemical industry. A computational framework for high-throughput screening and inverse design of high-performance MOFs for adsorption and membrane processes is proposed in this work. The framework offers guidelines for MOF design and is generically applicable to materials discovery for gas storage and separation.
NPJ COMPUTATIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Jia-Qi Wang, Rui-Lin He, Wen-Di Liu, Qi-Yun Feng, Yan-E Zhang, Chun-Yu Liu, Jing-Xuan Ge, Quan-Ming Wang
Summary: This article reports the synthesis and structure determination of chiral metal nanoclusters and investigates their potential in asymmetric catalysis. The incorporation of proline in the nanoclusters significantly enhances the catalytic efficiency in asymmetric reactions. This study demonstrates the promising application of metal nanoclusters in chiral catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Viveka K. Kulkarni, Behnam Nourmohammadi Khiarak, Shinjiro Takano, Sami Malola, Emily L. Albright, Tetyana Levchenko, Mark D. Aloisio, Cao-Thang Dinh, Tatsuya Tsukuda, Hannu Hakkinen, Cathleen M. Crudden
Summary: Researchers have successfully synthesized a previously unseen N-heterocyclic carbene-stabilized hydrido gold nanocluster and demonstrated its catalytic activity in the electrocatalytic reduction of CO2.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Sonu Kumar, Andrey Lyalin, Zhenguo Huang, Tetsuya Taketsugu
Summary: This study explores the catalytic activity and reaction pathway of oxygen functionalized hexagonal boron nitride (h-BN) in the oxidative dehydrogenation (ODH) of light alkanes. It is found that the synergy of >B-O-O-B< and >B-O-B< active sites at the zigzag edges of h-BN is crucial for the reaction. The ODH reaction temperature decreases with the increase in molecular mass of the light alkanes. The charge redistribution and localized oxygen atomic states during H-transfers provide possible descriptors for the design of new catalysts.
Article
Chemistry, Multidisciplinary
Haru Hirai, Shinjiro Takano, Takuya Nakashima, Takeshi Iwasa, Tetsuya Taketsugu, Tatsuya Tsukuda
Summary: In this study, a series of MAu12(dppe)(5)Cl-2 compounds with icosahedral structures were synthesized and their electronic structures, photoluminescence, and photocatalytic properties were systematically investigated. Doping an M element at the lower left of the periodic table expanded the energy gap between HOMO and LUMO, resulting in enhanced photoluminescence quantum yield. MAu12 (M=Pt, Rh, or Ir) exhibited higher photocatalytic activity than Au-13.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Masato Kobayashi, Yuta Oba, Tomoko Akama, Tetsuya Taketsugu
Summary: This paper proposes a practical electronic calculation method for lanthanide complexes, which introduces the frozen core potential approximation and relaxation of rotational degrees of freedom to improve the accuracy and convergence of the calculations.
JOURNAL OF MATHEMATICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Makoto Tsurui, Yuichi Kitagawa, Sunao Shoji, Hitomi Ohmagari, Miki Hasegawa, Masayuki Gon, Kazuo Tanaka, Masato Kobayashi, Tetsuya Taketsugu, Koji Fushimi, Yasuchika Hasegawa
Summary: A chiral Eu(III) coordination polymer with phase-transition behavior was studied to understand the effect of polymer chain arrangement on circularly polarized luminescence in a solid system. The phase transition of the polymer was characterized, and it was found that the CPL intensity changed drastically without changes in the coordination geometrical structure of the Eu(III) ion. This study demonstrates the orientation effect of a chiral Eu(III) coordination polymer on CPL properties in crystalline solids.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Review
Chemistry, Multidisciplinary
Takuro Tsutsumi, Yuriko Ono, Tetsuya Taketsugu
Summary: A method based on a reaction path network analysis is developed and applied to isomerization and bifurcation reactions of the Au-5 cluster. The method can construct a reduced-dimensionality reaction space, analyze dynamic reaction routes, and elucidate dynamic behaviors in reactions. It is a versatile tool with wide application value.
TOPICS IN CURRENT CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Takao Tsuneda, Hiroki Sumitomo, Masatoshi Hasebe, Takuro Tsutsumi, Tetsuya Taketsugu
Summary: It has been established that the reactive orbital energy theory (ROET) can theoretically reproduce the rule-based electronic theory diagrams of organic chemistry. By studying the charge transfer natures of typical organic carbon-carbon and carbon-heteroatom bond formation reactions, the ROET provides insights into the reactive orbitals and charge transferability indices. The ROET analyses also reveal the detailed orbital-based mechanisms for these reactions, explaining the pi-bond formations in acidic conditions and sigma-bond formations at alpha-carbons in basic conditions. Moreover, it is suggested that the methyl group plays a role in accepting and donating electrons in these reactions.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Masatsugu Nishida, Tomoko Akama, Masato Kobayashi, Tetsuya Taketsugu
Summary: In this study, a time-dependent Hartree-Fock-Bogoliubov (HFB) method is proposed for treating the excited states of molecules with static correlations at a reasonable computational cost. The canonical basis variant of the TDHFB method proposed by Ebata et al. is also considered to avoid electron number violations. Calculation results for the elongated hydrogen molecule show that the TDHFB method can partially incorporate two-electron excited determinants.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Hung Cuong Dinh, Ganesan Elumalai, Hidenori Noguchi, Andrey Lyalin, Tetsuya Taketsugu, Kohei Uosaki
Summary: In this study, the electrocatalytic activities of gold (Au) electrodes for the oxygen reduction reaction (ORR) were enhanced by modifying the Au surface with size-selected hexagonal boron nitride nanosheets (BNNS). The smaller the size of the BNNS, the lower the overpotential for ORR and the higher the ORR activity. The smallest BNNS size range (0.1-0.22 μm) reduced the overpotential by as much as 330 mV compared to a bare Au electrode, and it exhibited an ORR activity only 80 mV higher than that of a platinum (Pt) electrode.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Masatoshi Hasebe, Takuro Tsutsumi, Tetsuya Taketsugu, Takao Tsuneda
Summary: This study compares the effects of the long-range correction (LC) and CCSD method on the total and orbital electron densities of molecules. The LC stabilizes electrons in the long-range interaction regions of kinetic energy density, while the CCSD method stabilizes electrons in the long-range interaction regions in the vertical molecular planes. The LC has a similar effect to the CCSD method on unoccupied orbitals, but differs for occupied orbitals.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Keisuke Tashiro, Masato Kobayashi, Kiyotaka Nakajima, Tetsuya Taketsugu
Summary: A comprehensive reaction-path search using quantum chemical calculations was conducted to understand the mechanism of humin formation in the oxidation of HMF to FDCA. The study identified multiple reaction paths with low barriers for the reaction of HMF with OH-. It was also confirmed computationally that acetal protection of HMF could suppress humin formation.
Article
Chemistry, Multidisciplinary
Kewei Sun, Kazuma Sugawara, Andrey Lyalin, Yusuke Ishigaki, Kohei Uosaki, Oscar Custance, Tetsuya Taketsugu, Takanori Suzuki, Shigeki Kawai
Summary: In this study, complex organometallic oligomers were systematically synthesized on Cu(111) through sequential ring opening and bonding of phenanthroline derivatives by multiple Cu atoms. Characterization using scanning tunneling microscopy and density functional theory calculations revealed the role of Cu adatoms in the chiral oligomers. Furthermore, the strength of the bonds against sliding friction was found to be sufficient.
Article
Chemistry, Multidisciplinary
Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Tetsuya Taketsugu
Summary: Recently, surface-hopping ab initio molecular dynamics (SH-AIMD) simulations have been used to study the mechanisms and dynamics of excited-state chemical reactions. In this study, the authors investigate the effects of spin-orbit coupling (SOC) on the results of dynamics simulations using spin-pure and spin-mixed states for the hydride MH2 (M = Si, Ge, Sn, Pb). The results show that spin-mixed state potential energy surfaces are essential for simulating intersystem crossing in systems containing Sn and Pb elements.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Keijiro Toda, Yoshihiro Hirose, Emiko Kazuma, Yousoo Kim, Tetsuya Taketsugu, Takeshi Iwasa
Summary: Recent research investigated the photodissociation of the S-S bond of dimethyl disulfide (DMDS) using a scanning tunneling microscope with both far-and near-field light, showing that photodissociation at lower photon energies occurs in the near-field light compared to far-field light. The interaction with metal surfaces causes delocalization of the molecule's frontier orbitals, narrowing the HOMO-LUMO gap energy. Excited state distribution analysis revealed differences in electronic transitions between higher and lower excited states, with potential implications for the S-S bond dissociation reaction under different selection rules in near-field light.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
