Article
Chemistry, Multidisciplinary
Fabian Schlimpen, Tun Ast, Valerie Beneteau, Patrick Pale, Stefan Chassaing
Summary: A copper-catalysed three-component coupling reaction has been developed for the efficient synthesis of gamma-amino-ynamides. This method allows the use of simple starting materials and shows a broad functional group tolerance, making it a green and sustainable synthetic approach.
Article
Chemistry, Inorganic & Nuclear
Da Jin, Xiaofei Sun, Alexander Hinz, Peter W. Roesky
Summary: This article describes the synthesis and characterization of rare-earth metal complexes with redox-active formazanate ligands. Different types of complexes were obtained through protonation and salt metathesis reactions, and their electrochemical properties were studied using cyclic voltammetry.
DALTON TRANSACTIONS
(2022)
Article
Engineering, Chemical
Carmen Bacariza, Leila Karam, Nissrine El Hassan, Jose M. Lopes, Carlos Henriques
Summary: This study analyzed the effects of nickel loading, Si/Al ratio, and framework type on catalyst performance. Increasing nickel loading improved conversion rates but decreased stability. Si/Al ratio and zeolite type also had significant impacts on catalytic performance.
Article
Chemistry, Applied
Barbora Hudcova, Marek Osacky, Martina Vitkova, Aikaterini Mitzia, Michael Komarek
Summary: The study compared the adsorption efficiency and mechanisms of different types of zeolites for zinc (II), showing that synthetic zeolites had higher adsorption amount and binding strength than perlite by-product zeolites and natural zeolites, with natural zeolites mainly acting through cation exchange.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Physical
Marie E. Turano, Elizabeth A. Jamka, Maxwell Z. Gillum, K. D. Gibson, Rachael G. Farber, Weronika Walkosz, S. J. Sibener, Richard A. Rosenberg, Daniel R. Killelea
Summary: This passage discusses the high mobility of oxygen atoms on transition metal surfaces under demanding pressures and temperatures, leading to rapid surface diffusion, absorption into the subsurface, and reemergence on the surface. The unique role of subsurface oxygen atoms in the chemistry of oxidized metal catalysts is highlighted, but little is known about their formation and return to the surface. Additionally, localized changes in surface chemistry can occur due to oxygen diffusion between the surface and subsurface being mediated by defects.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Sung Hwan Park, Kingsley Christian Kemp, Jingeon Hong, Jung Gi Min, Suk Bong Hong
Summary: This study reveals that the ratio of alkali metal ions in synthesis mixtures is a critical parameter for successfully producing high-charge-density zeolite-like molecular sieves with various topologies, offering new opportunities for more efficient synthesis of novel zeolite structures.
Article
Chemistry, Inorganic & Nuclear
Samuel M. M. Bhutto, Brandon Q. Q. Mercado, Patrick L. L. Holland
Summary: In this study, the capability of iron(I) alkynyl complexes to bind N-2 was explored and a crystal structure of an iron(I) alkynyl complex with N-2 was obtained. It was further demonstrated that the alkynyl ligand is resistant to migration possibly due to the high Fe-C bond energy.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Sarah I. Allec, Manh-Thuong Nguyen, Roger Rousseau, Vassiliki-Alexandra Glezakou
Summary: The presence of bulk hydrogen significantly alters the electronic structure of the Ni(110) surface, leading to enhanced CO2 adsorption and reduction. This sheds light on a previously underappreciated mechanistic pathway for CO2 reduction on metal surfaces.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Energy & Fuels
Adelino F. Cunha, Sergio Morales-Torres, Luisa M. Pastrana-Martinez, Francisco J. Maldonado-Hodar, Nidia S. Caetano
Summary: The bimethanation of carbon dioxide using a Ni-catalyst supported on ZnO-doped 13X zeolite was studied. The results showed promising activities of the material, achieving CO2 conversions of 50-60% at high temperatures. Additionally, ZnO acted as an oxygen supplier in the presence of surface nickel.
Article
Chemistry, Physical
Florian Goltl, Saurabh Bhandari, Edgard A. Lebron-Rodriguez, Jake Gold, Stacey Zones, Ive Hermans, James A. Dumesic, Manos Mavrikakis
Summary: Cu-exchanged zeolites are potential materials for converting methane to methanol selectively. This study combines time dependent density functional theory with spin-orbit coupling to predict the optical spectra of Cu monomers and dimers in SSZ-13. The theoretical results are compared with experimental measurements, and the presence of Cu-hydroxy dimers and Cu monomers potentially explains the observed UV-vis-NIR spectra.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
M. Elsayed Moussa, E. -m. Rummel, G. Balazs, C. Riesinger, A. Noor, R. Kempe, M. Scheer
Summary: The reaction between (LCrCrL)-Cr-5 (L = N2C25H29, 1) and phosphaalkynes R-C P (R = tBu, Me, Ad) leads to the formation of neutral dimerization compounds [L2Cr2(mu,eta(1): eta(1): eta(2): eta(2)-P2C2R2)] (R = tBu (2), Me (3)) and tetrahedrane complex [L2Cr2(mu,eta(2): eta(2)-P = CAd)] (4). The 1,3-diphosphete ligands in complexes 2 and 3 exhibit a structural feature spanning a metal-metal multiple bond, while the larger adamantyl phosphaalkyne in compound 4 remains a monomer with side-on coordination mode.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Vikramjeet Singh, Abhishek Kundu, Kirti Singh, Debashis Adhikari
Summary: Formazan ligands have long been investigated as redox-noninnocent backbones, but their catalytic efficiency governed by redox noninnocence remains elusive. In this study, we report an iron-formazanate molecule that can efficiently prepare alpha-keto amides through a tightly regulated reductive cleavage of the substrate molecule by the electron donation from the formazanate, in a reversible manner.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Greggory T. Kent, Xiaojuan Yu, Guang Wu, Jochen Autschbach, Trevor W. Hayton
Summary: The reaction of [Cp3ThCl] with in situ generated 1-lithium-3,3-diphenylcyclopropene leads to the formation of [Cp3Th(3,3-diphenylcyclopropenyl)] (1), with good yields. Thermolysis of 1 results in isomerization to the ring-opened product, [Cp3Th(3-phenyl-1H-inden-1-yl)] (3) via a hypothesized carbene intermediate. This transformation represents a new reactivity mode of 3,3-diphenylcyclopropene with actinides, enhancing its utility as a carbene source. A combined DFT and C-13(H-1) NMR analysis of 1 reveals a spin-orbit induced downfield shift at C-alpha due to the involvement of 5f orbitals in the Th-C bond.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Mikalai A. Artsiusheuski, Rene Verel, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: Using in situ MAS NMR spectroscopy, the pathways of methane and methanol transformation over copper-containing mordenite were elucidated. Direct coupling of methane is not possible below 773 K, while the transformation of methanol and its partial oxidation products occur via the methanol-to-hydrocarbons (MTH) process. The presence of carbon monoxide leads to the formation of surface acetate species from methanol through the Koch carbonylation reaction, affecting the nature of the hydrocarbon pool species and the formed hydrocarbons.
Article
Chemistry, Multidisciplinary
Monika Kwoka, Elisabetta Comini, Dario Zappa, Jacek Szuber
Summary: This study compares the surface morphology and chemistry of flower-like ZnO nanostructures synthesized by thermal oxidation on native Si/SiO2 substrates using scanning electron microscopy (SEM), X-ray photoemission spectroscopy (XPS), and thermal desorption spectroscopy (TDS). SEM studies reveal that the nanostructures consist of isolated and irregular low-dimensional forms resembling rolled-up floss flowers and Liatris flowers with nanodendrites. XPS studies show slight surface nonstoichiometry and significant carbon surface contamination. TDS studies indicate that the undesired surface contaminations are only slightly removed, causing expected modifications in nonstoichiometry.
Review
Chemistry, Multidisciplinary
Nicholas F. Dummer, David J. Willock, Qian He, Mark J. Howard, Richard J. Lewis, Guodong Qi, Stuart H. Taylor, Jun Xu, Don Bethell, Christopher J. Kiely, Graham J. Hutchings
Summary: The direct transformation of methane to methanol at a larger scale remains challenging due to the low reactivity of methane. This review examines several promising routes to methanol and evaluates the performance targets necessary for process development. It provides critical perspectives on future operation and discusses the emergence of active heterogeneous catalysts and their reaction mechanisms.
Article
Astronomy & Astrophysics
Rong-Jun Liu, Jun Xu
Summary: Based on the well-calibrated IBUU transport model, the dynamical effect of incorporating rigorous angular momentum conservation in each collision of particles has been studied. Two typical prescriptions were compared with the original one for handling the constraint of rigorous angular momentum conservation. Although the results depend quantitatively on the choice of the prescription, it was found that angular momentum conservation generally reduces local density fluctuations, collision rate, and may have an influence on density evolution, collective flow, and pion production in transport simulations of intermediate-energy heavy-ion collisions.
Article
Chemistry, Multidisciplinary
Wei Gao, Qiang Wang, Guodong Qi, Jiawei Liang, Chao Wang, Jun Xu, Feng Deng
Summary: By using 1D Mo-95 NMR and 2D H-1-Mo-95 heteronuclear correlation solid-state NMR spectroscopy, the active ensembles in the confined channels of Mo/ZSM-5 zeolite during the MDA reaction were observed. Two kinds of MoOxCy species were identified, with MoOxCy-II showing higher activity for methane activation and benzene formation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Vinicius Martins, Bryan E. G. Lucier, Kuizhi Chen, Ivan Hung, Zhehong Gan, Christel Gervais, Christian Bonhomme, Heng-Yong Nie, Wanli Zhang, Yining Huang
Summary: Porous metal-organic frameworks (MOFs) have diverse applications in various fields, and post synthetic modification (PSM) approaches can enhance their properties. In this study, high-field solid-state NMR techniques were used to gain molecular-level insights into a prototypical aluminum MOF and its interactions with metal guests. The results provide detailed information about the oxygen environment, intermolecular interactions, and host-guest connectivity in the MOF.
CHEMISTRY OF MATERIALS
(2023)
Article
Astronomy & Astrophysics
Lu-Meng Liu, Jun Xu, Guang-Xiong Peng
Summary: The possibility of using free spectator nucleons in central tip-tip and body-body collisions to extract the information of the deformed neutron skin in four typical deformed nuclei was explored. It was found that the polar angular distributions of the neutron skin in 96Ru and 197Au can be extracted by comparing the yield ratios of free spectator neutrons to protons in their central tip-tip and body-body collisions.
Review
Chemistry, Multidisciplinary
Xin Chang, Yu-Ming Zhao, Boheng Yuan, Min Fan, Qinghai Meng, Yu-Guo Guo, Li-Jun Wan
Summary: The energy crisis and environmental pollution have led to increased focus on renewable energy development and utilization. However, due to the unpredictable nature of renewable energy resources, energy storage systems are needed to collect and release electricity during peak periods. Among various energy storage technologies, lithium-ion batteries are preferred due to their flexible power and energy, quick response, and high energy conversion efficiency. This review evaluates the priorities and challenges of traditional lithium-ion batteries in grid energy storage, and discusses the potential of solid-state lithium-ion batteries as an alternative with superior performance and safety. The challenges of developing solid-state lithium-ion batteries, such as low ionic conductivity of the electrolyte, unstable electrode/electrolyte interface, and complicated fabrication process, are also discussed.
SCIENCE CHINA-CHEMISTRY
(2023)
Article
Chemistry, Physical
Weiyu Wang, Qiang Wang, Jun Xu, Feng Deng
Summary: Parahydrogen-induced polarization (PHIP) is a technique that can increase the NMR sensitivity by several orders. It is a powerful tool to characterize catalyst properties and elucidate reaction mechanisms. In this Perspective, the heterogeneous PHIP (HET-PHIP) technique and its application in catalytic hydrogenation are comprehensively reviewed. The fundamentals of HET-PHIP are introduced and its ability to provide information about catalyst morphology and electronic properties is discussed. The mechanistic understanding of catalytic hydrogenations using HET-PHIP is also discussed.
Article
Chemistry, Physical
Qiang Ma, Sha Fu, An-Jun Wu, Qi Deng, Wei-Dong Li, Dan Yue, Bing Zhang, Xiong-Wei Wu, Zhen-Ling Wang, Yu-Guo Guo
Summary: Bidirectionally functional polymer electrolytes (BDFPE) were designed to simultaneously handle the interface issues faced by anodes and cathodes. By constructing the BDFPE, a smooth and dendrite-free lithium deposition is enabled for Li||Li symmetry cells, and Li||LiNi0.6Co0.2Mn0.2O2 batteries demonstrate favorable cycling and rate capability with a stable CEI layer. The study provides a promising design strategy for high energy density lithium metal batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Yanan Xu, Kai Wang, Xudong Zhang, Yibo Ma, Qifan Peng, Yue Gong, Sha Yi, Hua Guo, Xiong Zhang, Xianzhong Sun, Hongcai Gao, Sen Xin, Yu-Guo Guo, Yanwei Ma
Summary: A 10-nm polydopamine coating on the residue-removed garnet surface is shown to stabilize the modified garnet filler and prevent the generation of alkaline residues, allowing PVDF to remain intact. Metal-nitrogen bonding between the La atoms of garnet and the amino groups of polydopamine promotes stronger adsorption of Li ions, enabling an efficient ion-percolation network for Li-ion conduction through the garnet-polydopamine interface. The composite electrolyte demonstrates an effective room-temperature Li+ conductivity of 1.52 x 10(-4) S cm(-1) and a high cutoff voltage of up to 4.7 V versus Li+/Li to support stable operation of all-solid-state Li-LiCoO2 batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Jing Niu, Yu-Ting Miao, Wei David Wang, Meng-Tong Ruan, Zhi-Peng Wang, Hua-Dong Xue, Si-Min Yu, Chong Liu, Jian-Feng Wu, Wei Wang
Summary: The crucial role of surface ethoxy species, i.e., equilibrium with ethene in the primary step and further alkylation to form the C-C bond, was confirmed for the first time through a selective C-13-labeling protocol and a multitechnique approach during the adsorption of ethene on zeolite H-Y.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Xiang Wang, Shuangqin Zeng, Guodong Qi, Qiang Wang, Jun Xu, Feng Deng
Summary: A Pt/Al2O3 catalyst was prepared on pentahedral Al-rich Al2O3, allowing the embedding of Pt nanoparticles into the support. The embedded Pt nanoparticles exhibited improved CO oxidation performance compared to surface Pt species at suitable GHSV, providing a promising approach to tune the properties of supported Pt catalysts.
CHEMICAL COMMUNICATIONS
(2023)
Article
Physics, Nuclear
Lei-Ming Hua, Jun Xu
Summary: Based on Boltzmann-Uehling-Uhlenbeck simulations calibrated by the transport model evaluation project, this study investigates the specific shear viscosity q/s of nuclear matter in the spinodal region using the Green-Kubo method. By utilizing a momentum-independent mean-field potential that reproduces empirical nuclear matter properties and the nuclear phase diagram, stable and thermalized nuclear cluster systems are generated in a box with periodic boundary conditions. Extensive comparisons of q/s at different densities and temperatures in uniform and nonuniform systems reveal that the shear viscosity is smaller in nuclear clusters due to enhanced correlation of the energy-momentum tensor and stronger collision effects. The temperature dependence of q/s exhibits a minimum only at low average densities (p < 0.3p0). This study provides a rigorous baseline calculation of q/s in nuclear systems with clusters and enhances our understanding of the relationship between shear viscosity and the nuclear phase diagram.
Article
Chemistry, Physical
Weiyu Wang, Qiang Wang, Jun Xu, Feng Deng
Summary: Parahydrogen-induced polarization (PHIP) is an NMR hyperpolarization technique that enhances NMR sensitivity. This technique generates hyperpolarization through pairwise addition behavior, making it useful for catalyst characterization and understanding reaction mechanisms. This Perspective provides a comprehensive overview of the heterogeneous PHIP (HET-PHIP) technique and its applications in catalytic hydrogenation. The fundamentals of HET-PHIP are introduced, along with its ability to provide information about catalyst morphology and electronic properties. The paper also discusses advancements in mechanistic understanding achieved using HET-PHIP and the limitations and prospects of this technique.
Article
Chemistry, Multidisciplinary
Chao Wang, Yueying Chu, Danfeng Xiong, Haifeng Wang, Min Hu, Qiang Wang, Jun Xu, Feng Deng
Summary: We investigate the role of water in benzene methylation over ZSM-5 zeolite using solid-state NMR experiments and theoretical simulations. We find that water competes with benzene for the active sites of the zeolite and facilitates the reaction mechanism. The growth of water clusters induces a micro-hydrophobic effect in zeolite pores, which reorients benzene molecules and promotes their interactions with surface methoxy species on the zeolite.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)