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Atomically Dispersed Iron-Copper Dual-Metal Sites Synergistically Boost Carbonylation of Methane

Angewandte Chemie 2024年第43期136卷

作者： Dr. Qingpeng Cheng Dr. Xueli Yao Prof. Dr. Guanna Li Guanxing Li Prof. Dr. Lirong Zheng Dr. Kaijie Yang Dr. Abdul-Hamid Emwas Prof. Dr. Xingang Li Prof. Dr. Yu Han Prof. Dr. Jorge Gascon KAUST Catalysis Center (KCC) Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Biobased Chemistry and Technology Wageningen University & Research Bornse Weilanden 9 Wageningen 6708WG The Netherlands Advanced Membranes and Porous Materials Center (AMPMC) KAUST Thuwal 23955-6900 Saudi Arabia Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Imaging and Characterization Core Lab KAUST Thuwal 23955-6900 Saudi Arabia State Key Laboratory of Chemical Engineering Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Haihe Laboratory of Sustainable Chemical Transformations Tianjin Key Laboratory of Applied Catalysis Science and Engineering School of Chemical Engineering & Technology Tianjin University Tianjin 300350 P. R. China Electron Microscopy Center School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P. R. China

The direct liquid-phase oxidative carbonylation of methane, utilizing abundant natural gas, offers a mild and straightforward alternative. However, most catalysts proposed for this process suffer from low acetic acid yields due to few active sites and rapid C1 oxygenate generation, impeding their industrial feasibility. Herein, we report a highly efficient 0.1Cu/Fe-HZSM-5-TF (TF denotes template-free synthesis) catalyst featuring exclusively mononuclear Fe and Cu anchored in the ZSM-5 channels. Under optimized conditions, the catalyst achieved an unprecedented acetic acid yield of 40.5 mmol g cat −1 h −1 at 50 °C, tripling the previous records of 12.0 mmol g cat −1 h −1 . Comprehensive characterization, isotope-labeled experiments and density functional theory (DFT) calculations reveal that the homogeneous mononuclear Fe sites are responsible for the activation and oxidation of methane, while the neighboring Cu sites play a key role in retarding the oxidation process, promoting C−C coupling for effective acetic acid synthesis. Furthermore, the methyl-group carbon in acetic acid originates solely from methane, while its carbonyl-group carbon is derived exclusively from CO, rather than the conversion of other C1 oxygenates. The proposed bimetallic catalyst design not only overcomes the limitations of current catalysts but also generalizes the oxidative carbonylation of other alkanes, demonstrating promising advancements in sustainable chemical synthesis.

关键词： Methane oxidation Carbonylation Zeolites C1 chemistry synergy

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Separation and recovery of vanadium from leaching solution of calcium roasting vanadium slag by extraction with P204 extractant

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Minerals Engineering 2025年 232卷

作者： Da-long Wang Lin Zhang Jing-wei Li Chen Chen Yin-he Lin Zhi Yang Da-ya Wang Huan-jian Hou Jian Chen Tang-jie Zhou Wen-ming Tang Engineering Research Center of High Performance Copper Alloy Materials and Processing Ministry of Education & School of Materials Science and Engineering Hefei University of Technology Hefei 230009 Anhui China Pangang Group Xichang Vanadium Products Technology Co. LTD Xichang 615000 China School of Mechanical Engineering Tongling University Tongling 244061 China School of Chemistry and Chemical Engineering Yangtze Normal University Fuling 408100 Chongqing China Sinosteel Maanshan General Institute of Mining Research Co. Ltd. The National Engineering Technology Research Center of Solid Waste Treatment and Disposal for Metal Mines Maanshan Anhui 243000 China Institute of Solid State Physics Hefei Institutes of Physical Science Chinese Academy of Sciences Hefei 230031 China

In this study, an efficient method for recovery of vanadium (V) from leaching solution of calcium roasting vanadium slag by extraction with di(2-ethylhexyl) phosphate (P204) was proposed. The impact of initial pH value, P204 concentration, contact time, phase ratio (O/A) and temperature on vanadium recovery were analyzed. The effects of stripping agent, O/A, contact time and temperature on the V stripping were analyzed. The maximum V extraction rate was 99.74 % through three-stage extraction under the conditions: 50 % P204, O/A of 1:1, pH of 4.0, 8 min, 30℃. The three-stage maximum vanadium stripping rate was 98.38 % under the conditions of 2.5 M H 2 SO 4 solution, 10 min, 30 ℃. The purity of the recovered V 2 O 5 was 99.59 % when the pH value was 2.0. The extraction mechanism of vanadium was confirmed as cation exchange mechanism by using Fourier transform infrared spectroscopy.

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Gapped and Rotated Grain Boundary Revealed in Ultra-Small Au Nanoparticles for Enhancing Electrochemical CO2Reduction

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Angewandte Chemie 2024年第3期137卷

作者： Wenying Wang Dr. Dong Chen Dr. Victor Fung Dr. Shengli Zhuang Yue Zhou Dr. Chengming Wang Guoqing Bian Dr. Yan Zhao Dr. Nan Xia Prof. Dr. Jin Li Prof. Dr. Haiteng Deng Dr. Lingwen Liao Prof. Dr. Jun Yang Prof. Dr. De-en Jiang Prof. Dr. Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and Nanotechnology CAS Center for Excellence in Nanoscience Institute of Solid State Physics HFIPS Chinese Academy of Sciences 230031 Hefei P. R. China Key Laboratory of Precision and Intelligent Chemistry University of Science and Technology of China 230026 Hefei P. R. China State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences 100190 Beijing P. R. China Department of Chemistry University of California 92521 Riverside CA USA School of Computational Science and Engineering Georgia Institute of Technology 30332 Atlanta Georgia USA Institute of Physical Science and Information Technology Anhui University 230601 Hefei P. R. China Instruments' Center for Physical Science University of Science and Technology of China 230026 Hefei P. R. China Tsinghua University-Peking University Joint Center for Life Sciences School of Life Sciences Tsinghua University 100084 Beijing P. R. China MOE Key Laboratory of Bioinformatics School of Life Sciences Tsinghua University 100084 Beijing P. R. China Department of Chemical and Biomolecular Engineering Vanderbilt University 37235 Nashville Tennessee USA

Although gapped grain boundaries have often been observed in bulk and nanosized materials, and their crucial roles in some physical and chemical processes have been confirmed, their acquisition at ultrasmall nanoscale presents a significant challenge. To date, they had not been reported in metal nanoparticles smaller than 2 nm owing to the difficulty in characterization and the high instability of grain boundary (GB) atoms. Herein, we have successfully developed a synthesis method for producing a novel chiral nanocluster Au 78 (TBBT) 40 (TBBT=4-tert-butylphenylthiolate) with a 26-atom gapped and rotated GB. This nanocluster was precisely characterized using single-crystal X-ray crystallography and mass spectrometry. Additionally, an offset atomic defect linked to the peripheral Au(TBBT) 2 staple was found in the structure. Comparing it to similarly face-centered cubic-structured Au 36 (TBBT) 24 , Au 44 (TBBT) 28 , Au 52 (TBBT) 32 , Au 92 (TBBT) 44 , and ~5 nm nanocrystals, the bridging Au 78 (TBBT) 40 nanocluster exhibited higher catalytic activity in the electroreduction of CO 2 to CO. This enhanced activity was explained through density functional theory calculations and X-ray photoelectron spectroscopy analysis, which highlight the impact of GBs and point defects on the surface properties of metal nanoclusters in balancing intermediate adsorption and product desorption.

关键词： Au78(TBBT)40 Grain boundary CO2 reduction reaction

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Critical pore radius and transport properties of disordered hard- And overlapping-sphere models

arXiv

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arXiv 2021年

作者： Klatt, Michael A. Ziff, Robert M. Torquato, Salvatore Department of Physics Princeton University PrincetonNJ08544 United States Institut für Theoretische Physik FAU Erlangen-Nürnberg Staudtstr. 7 Erlangen91058 Germany Center for the Study of Complex Systems Department of Chemical Engineering University of Michigan Ann ArborMI48109 United States Department of Physics Princeton University PrincetonNJ08544 United States Department of Chemistry Princeton Institute for the Science and Technology of Materials Program in Applied and Computational Mathematics Princeton University PrincetonNJ08544 United States

Transport properties of porous media are intimately linked to their pore-space microstructures. We quantify geometrical and topological descriptors of the pore space of certain disordered and ordered distributions of spheres, including pore-size functions and the critical pore radius δc. We focus on models of porous media derived from maximally random jammed sphere packings, overlapping spheres, equilibrium hard spheres, "quantizer" sphere packings, and crystalline sphere packings. For precise estimates of the percolation thresholds, we use a strict relation of the void percolation around sphere configurations to weighted bond percolation on the corresponding Voronoi networks. We use the Newman-Ziff algorithm to determine the percolation threshold using universal properties of the cluster size distribution. The critical pore radius δc is often used as the key characteristic length scale that determines the fluid permeability k. A recent study [Torquato. Adv. Wat. Resour. 140,103565 (2020)] suggested for porous media with a well-connected pore space an alternative estimate of k based on the second moment of the pore size hδ2i, which is easier to determine than δc. Here, we compare δc to the second moment of the pore size hδ2i, and indeed confirm that, for all porosities and all models considered, δc2 is to a good approximation proportional to hδ2i. However, unlike hδ2i, the permeability estimate based on δc2 does not predict the correct ranking of k for our models. Thus, we confirm hδ2i to be a promising candidate for convenient and reliable estimates of the fluid permeability for porous media with a well-connected pore space. Moreover, we compare the fluid permeability of our models with varying degrees of order, as measured by the τ order metric. We find that (effectively) hyperuniform models tend to have lower values of k than their nonhyperuniform counterparts. Our findings could facilitate the design of porous media with desirable transport properties via target

关键词： Porous materials

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Ab initio Derivation of Low-Energy Hamiltonians for Systems with Strong Spin-Orbit Interaction and Its Application to Ca5Ir3O12

arXiv

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arXiv 2021年

作者： Charlebois, Maxime Moree, Jean-Baptiste Nakamura, Kazuma Nomura, Yusuke Tadano, Terumasa Yoshimoto, Yoshihide Yamaji, Youhei Hasegawa, Takumi Matsuhira, Kazuyuki Imada, Masatoshi Waseda Research Institute for Science and Engineering Waseda University Okubo Shinjuku Tokyo169-8555 Japan Kyushu Institute of Technology Graduate School of Engineering Kitakyushu804-8550 Japan Riken Center for Emergent Matter Science 2-1 Hirosawa Wako Saitama351-0198 Japan Research Center for Magnetic and Spintronic Materials National Institute for Materials Science Tsukuba305-0047 Japan Department of Computer Science University of Tokyo 7-3-1 Hongo Bunkyo-ku Tokyo113-0033 Japan Department of Applied Physics University of Tokyo Hongo Bunkyo-ku Tokyo113-8656 Japan Graduate School of Integrated Arts and Sciences Hiroshima University Higashihiroshima Hiroshima739-8521 Japan Toyota Physical and Chemical Research Institute Yokomichi Nagakute Aichi480-1118 Japan

We present an ab initio derivation method for e_ective low-energy Hamiltonians of material with strong spin-orbit interactions. The e_ective Hamiltonian is described in terms of the Wannier function in the spinor form, and e_ective interactions are derived with the constrained random phase approximation (cRPA) method. Based on this formalism and the developed code, we derive an e_ective Hamiltonian of a strong spin-orbit interaction material Ca5Ir3O12. This system consists of three edge-shared IrO6 octahedral chains arranged along the c axis, and the three Ir atoms in the ab plane compose a triangular lattice. For such a complicated structure, we need to set up the Wannier spinor function under the local coordinate system. We found that a density-functional band structure near the Fermi level is formed by local dxy and dyz orbitals. Then, we constructed the ab initio dxy=dyz model. The estimated nearest neighbor transfer t is close to 0.2 eV, and the cRPA onsite U and neighboring V electronic interactions are found to be 2.4-2.5 eV and 1 eV, respectively. The resulting characteristic correlation strength de_ned by (U ô V )=t is above 7, and thus this material is classi_ed as a strongly correlated electron system. The onsite transfer integral involved in the spin-orbit interaction is 0.2 eV, which is comparable to the onsite exchange integrals_0.2 eV, indicating that the spin-orbit-interaction physics would compete with the Hund physics. Based on these calculated results, we discuss possible rich ground-state low-energy electronic structures of spin, charge and orbitals with competing Hund, spin-orbit and strong correlation physics. © 2021, CC BY.

关键词： Hamiltonians

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Superfluidity and pairing phenomena in ultracold atomic Fermi gases in one-dimensional optical lattices, Part II: Effects of population imbalance

arXiv

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arXiv 2020年

作者： Wang, Jibiao Sun, Lin Zhang, Qiang Zhang, Leifeng Yu, Yi Lee, Chaohong Chen, Qijin Zhuhai Guangdong519082 China Department of Physics Zhejiang Institute of Modern Physics Zhejiang University Hangzhou Zhejiang310027 China College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang310014 China Guangzhou Guangdong510275 China Shanghai Branch National Laboratory for Physical Sciences at Microscale Department of Modern Physics University of Science and Technology of China Shanghai201315 China Synergetic Innovation Center of Quantum Information and Quantum Physics Hefei Anhui230026 China

In this paper, we study the effect of population imbalance and its interplay with pairing strength and lattice effect in atomic Fermi gases in a one-dimensional optical lattice. We compute various phase diagrams as the system undergoes BCS-BEC crossover, using the same pairing fluctuation theory as in Part I. We find widespread pseudogap phenomena beyond the BCS regime and intermediate temperature superfluid states for relatively low population imbalances. The Fermi surface topology plays an important role in the behavior of Tc. For large d and/or small t, which yield an open Fermi surface, superfluidity can be readily destroyed by a small amount of population imbalance p. The superfluid phase, especially in the BEC regime, can exist only for a highly restricted volume of the parameter space. Due to the continuum-lattice mixing, population imbalance gives rise to a new mechanism for pair hopping, as assisted by excessive majority fermions, which may lead to significant enhancement of Tc on the BEC side of the Feshbach resonance, and also render Tc approaching a constant asymptote in the BEC limit, when it exists. Furthermore, we find that not all minority fermions will be paired up in BEC limit, unlike the 3D continuum case. These predictions can be tested in future experiments. Copyright © 2020, The Authors. All rights reserved.

关键词： Fermions

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What's knot to like? Observation of a linked loop quantum state

arXiv

引用

arXiv 2021年

作者： Belopolski, Ilya Chang, Guoqing Cochran, Tyler A. Cheng, Zi-Jia Yang, Xian P. Hugelmeyer, Cole Manna, Kaustuv Yin, Jia-Xin Cheng, Guangming Multer, Daniel Litskevich, Maksim Shumiya, Nana Zhang, Songtian S. Shekhar, Chandra Schröter, Niels B.M. Chikina, Alla Polley, Craig Thiagarajan, Balasubramanian Leandersson, Mats Adell, Johan Huang, Shin-Ming Yao, Nan Strocov, Vladimir N. Felser, Claudia Zahid Hasan, M. Department of Physics Princeton University Princeton NJ08544 United States Saitama Wako351-0198 Japan Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 21 Nanyang Link 637371 Singapore Department of Mathematics Princeton University Princeton NJ08544 United States Max Planck Institute for Chemical Physics of Solids Nöthnitzer Straße 40 Dresden01187 Germany Department of Physics Indian Institute of Technology Delhi Hauz Khas New Delhi110016 India Princeton Institute for Science and Technology of Materials Princeton University Princeton NJ08544 United States Swiss Light Source Paul Scherrer Institut Villigen CH-5232 Switzerland MAX IV Laboratory Lund University P.O. Box 118 Lund221 00 Sweden Department of Physics National Sun Yat-Sen University Kaohsiung804 Taiwan Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States

Quantum phases can be classified by topological invariants, which take on discrete values capturing global information about the quantum state [1-19]. Over the past decades, these invariants have come to play a central role in describing matter, providing the foundation for understanding superfluids [6, 7], magnets [8, 9], the quantum Hall effect [4, 10], topological insulators [11-15], Weyl semimetals [16-19] and other phenomena. Here we report a remarkable linking number (knot theory) invariant associated with loops of electronic band crossings in a mirror-symmetric ferromagnet [20-26]. Using state-of-the-art spectroscopic methods, we directly observe three intertwined degeneracy loops in the material's bulk Brillouin zone three-torus, T3. We find that each loop links each other loop twice. Through systematic spectroscopic investigation of this linked loop quantum state, we explicitly draw its link diagram and conclude, in analogy with knot theory, that it exhibits linking number (2, 2, 2), providing a direct determination of the invariant structure from the experimental data. On the surface of our samples, we further predict and observe Seifert boundary states protected by the bulk linked loops, suggestive of a remarkable Seifert bulk-boundary correspondence. Our observation of a quantum loop link motivates the application of knot theory to the exploration of exotic properties of quantum matter. © 2021, CC BY.

关键词： Graph theory

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Superfluidity and pairing phenomena in ultracold atomic Fermi gases in one-dimensional optical lattices, Part I: Balanced case

arXiv

引用

arXiv 2020年

作者： Wang, Jibiao Zhang, Leifeng Yu, Yi Lee, Chaohong Chen, Qijin Zhuhai Guangdong519082 China Department of Physics Zhejiang Institute of Modern Physics Zhejiang University Hangzhou Zhejiang310027 China College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang310014 China Guangzhou Guangdong510275 China Shanghai Branch National Laboratory for Physical Sciences at Microscale Department of Modern Physics University of Science and Technology of China Shanghai201315 China Synergetic Innovation Center of Quantum Information and Quantum Physics Hefei Anhui230026 China

The superfluidity and pairing phenomena in ultracold atomic Fermi gases have been of great interest in recent years, with multiple tunable parameters. Here we study the BCS-BEC crossover behavior of balanced two-component Fermi gases in a one-dimensional optical lattice, which is distinct from the simple three-dimensional (3D) continuum and a fully 3D lattice often found in a condensed matter system. We use a pairing fluctuation theory which includes self-consistent feedback effects at finite temperatures, and find widespread pseudogap phenomena beyond the BCS regime. As a consequence of the lattice periodicity, the superfluid transition temperature Tc decreases with pairing strength in the BEC regime, where it approaches asymptotically Tc = πan/2m, with a being the s-wave scattering length, and n (m) the fermion density (mass). In addition, the quasi-two dimensionality leads to fast growing (absolute value of the) fermionic chemical potential µ and pairing gap ∆, which depends exponentially on the ratio d/a. Importantly, Tc at unitarity increases with the lattice constant d and hopping integral t. The effect of the van Hove singularity on Tc is identified. The superfluid density exhibits T3/2 power laws at low T, away from the extreme BCS limit. These predictions can be tested in future experiments. Copyright © 2020, The Authors. All rights reserved.

关键词： Optical lattices

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Real-Space imaging of the ordered small molecule orientations in porous frameworks by electron microscopy

arXiv

引用

arXiv 2020年

作者： Shen, Boyuan Chen, Xiao Cai, Dali Xiong, Hao Jin, Shifeng Liu, Xin Han, Yu Wei, Fei Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Beijing100084 China Research and Development Center for Functional Crystals Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China School of Chemistry Dalian University of Technique Dalian116024 China KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Thuwal23955-6900 Saudi Arabia Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Thuwal23955-6900 Saudi Arabia

The real-space imaging of small molecules is always challenging under the electron microscopes, but highly demanded for investigating various nanoscale interactions, such as hydrogen bond and van der Waals (vdW) force1-6. Especially, identifying the host-guest interactions in porous materials directly at the molecular level will bring a deeper insight into the behaviors of guest molecules during the sorption, catalysis, gas separation and energy storage. In this work, we directly resolved the ordered configurations of p-xylenes (PXs) adsorbed in ZSM-5 frameworks by the scanning transmission electron microscopy (STEM) with the integrated differential phase contrast (iDPC) technique7-10 to identify the host-guest vdW interactions. Based on these observations, we revealed that the PXs in one straight channel modified the channel geometry with a coherent orientation. And the adjacent straight channels were deformed up to 8.8% along the different directions corresponding to three dominant PX configurations, resulting a negligible overall expansion of ZSM-5 lattices. Then, we could also image the disorder and desorption of PXs in ZSM-5 channels during the in situ heating. This work not only helped us to study the host-guest vdW interactions and the sorption behaviors of PXs in ZSM-5, but also provided an efficient tool for further imaging and studying other single-molecule behaviors under STEMs. Copyright © 2020, The Authors. All rights reserved.

关键词： Van der Waals forces

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The Effect of the Polyaromatic Hydrocarbon in the Formation of Fullerenes

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Advanced Materials 2020年第10期59卷 3970-3975页

作者： Wu, Bo Jiang, Li Luo, Yi Wang, Chunru Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and Nanotecnology Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street No. 2 Beijing100190 China Hefei National Laboratory for Physical Sciences at the Microscale Department of Chemical Physics Synergetic Innovation Center of Quantum Information and Quantum Physics University of Science and Technology of China Hefei Anhui230026 China Department of Theoretical Chemistry School of Biotechnology Royal Institute of Technology AlbaNova Stockholm10691 Sweden

Tremendous advances in nanoscience have been made since the discovery of fullerenes. However, the short timescale of the growth process and high-energy conditions of synthesis result in severe constraints to investigation of the mechanism of fullerene formation. In this work, we attempted to reveal the formation process by analyzing the variation in the yield of fullerenes under different conditions. Experiments and theoretical analysis show that the formation of fullerenes could be affected by the addition of polycyclic aromatic compounds. It is proposed that the formation of C60 during arcdischarge synthesis is fragment assembling, while the yield of C2m (m=35, 38, 39) is strongly enhanced by building-block splicing. In addition, several features of the building blocks are put forward to predict the extent of their influence to the formation of larger fullerenes C2n (n ≥ 42). This work not only provides essential insight into the formation process of fullerenes, but more importantly also paves the way to improving the yield of larger fullerenes selectively. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

关键词： Fullerenes

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