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Titelbild: Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering (Angew. Chem. 45/2024)

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Angewandte Chemie 2024年第45期136卷

作者： Junwei Bian Wei Zhang Prof. Yun Hau Ng Prof. Zhuofeng Hu Prof. Zhen Wei Yuxi Liu Prof. Jiguang Deng Prof. Hongxing Dai Prof. Lin Jing Beijing Key Laboratory for Green Catalysis and Separation College of Materials Science and Engineering Beijing University of Technology Beijing 100124 China School of Energy and Environment City University of Hong Kong Tat Chee Avenue Kowloon 999077 Hong Kong S.A.R. China Chemical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal 23955-6900 Kingdom of Saudi Arabia School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510275 China

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High-temperature mid-IR absorption and reaction kinetics of 2-methyl-1,3-dioxolane: An experimental and theoretical study

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Journal of Photochemistry and Photobiology 2023年 13卷

作者： Adil, Mohammad Giri, Binod Raj Mai, Tam V.-T. Szőri, Milán Huynh, Lam K. Farooq, Aamir Mechanical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia KAUST Clean Combustion Research Center King Abdullah University of Science and Technology Saudi Arabia Molecular Science and Nano-Materials Lab Institute for Computational Science and Technology SBI Building Quang Trung Software City Tan Chanh Hiep Ward District 12 Ho Chi Minh Viet Nam University of Science Vietnam National University – HCMC 227 Nguyen Van Cu Ward 4 District 5 Ho Chi Minh Viet Nam Vietnam National University – HCMC Quarter 6 Linh Trung Ward Thu Duc Ho Chi Minh Viet Nam Institute of Chemistry University of Miskolc Egyetemváros A/2 Miskolc H-3515 Hungary School of Chemical and Environmental Engineering International University Quarter 6 Linh Trung Ward Thu Duc City Ho Chi Minh City Viet Nam

This work reports the mid-IR spectroscopy and reaction kinetics of 2-methyl-1,3-dioxolane (2M13DO). We carried out spectroscopic measurements to deduce temperature-dependent absorption cross-sections of 2M13DO over a broad wavelength range of 8.4–10.5 μm (950–1190 cm⁻¹). For these measurements, we employed a rapidly tuning MIRcat-QT™ laser that can be operated either at a fixed wavelength or scanned mode over wide wavelength regions. By operating the laser at a fixed wavelength, we monitored the decay of 2M13DO behind reflected shock waves over T₅ = 1050–1400 K and P₅ = 0.7 and 2.6 bar. Our measured concentration time-histories of 2M13DO allowed us to directly extract the overall rate coefficients for the unimolecular decomposition of 2M13DO using the first-order rate law. We did not observe any pressure dependence in the measured rate coefficients, indicating that the reaction is close to the high-pressure limit. By employing the W1U composite method, we explored the important pyrolysis reaction pathways of 2M13DO in the reactive potential energy surface. Three important reaction channels, namely, 2M13DO → CH₂[dbnd]CHOCH₂CH₂OH (IM1), 2M13DO → 2CH₃CHO (P3), 2M13DO → CH₃ + 1,3-dioxolan-2-yl (P4) were identified. Below 700 K, IM1 forming channel is dominant, whereas CH₃CHO formation is dominant under our experimental conditions. Above 1500 K, the radical forming channel (CH₃+P4) takes over other channels. At higher temperatures, the contribution of the radical forming channel continually increases, accounting for ∼ 99% at 2000 K. We used the stochastic RRKM-ME model to predict the pressure and temperature dependence of the rate coefficients, k(T, P), and time-resolved species profiles. Our theory showed excellent agreement with the measured rate coefficients. These are the first direct determination of the rate coefficients of the unimolecular decomposition of

关键词： 2-Methyl-1,3-dioxolane Absorption spectra High-temperature Pyrolysis RRKM-ME calculations Shock tube

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Observation of the dual quantum spin Hall insulator by density-tuned correlations in a van der Waals monolayer

arXiv

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arXiv 2024年

作者： Tang, Jian Ding, Thomas Siyuan Chen, Hongyu Gao, Anyuan Qian, Tiema Huang, Zumeng Sun, Zhe Han, Xin Strasser, Alex Li, Jiangxu Geiwitz, Michael Shehabeldin, Mohamed Belosevich, Vsevolod Wang, Zihan Wang, Yiping Watanabe, Kenji Taniguchi, Takashi Bell, David C. Wang, Ziqiang Fu, Liang Zhang, Yang Qian, Xiaofeng Burch, Kenneth S. Shi, Youguo Ni, Ni Chang, Guoqing Xu, Su-Yang Ma, Qiong Department of Physics Boston College Chestnut HillMA United States Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore Singapore Department of Chemistry and Chemical Biology Harvard University CambridgeMA United States Department of Physics and Astronomy and California NanoSystems Institute University of California Los Angeles Los AngelesCA United States Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing China Department of Materials Science and Engineering Texas A&M University College StationTX United States Department of Physics and Astronomy University of Tennessee KnoxvilleTN United States Min H. Kao Department of Electrical Engineering and Computer Science University of Tennessee KnoxvilleTN United States Research Center for Electronic and Optical Materials National Institute for Materials Science Tsukuba Japan Research Center for Materials Nanoarchitectonics National Institute for Materials Science Tsukuba Japan Harvard John A. Paulson School of Engineering and Applied Sciences The Center for Nanoscale system Harvard University CambridgeMA United States Department of Physics Massachusetts Institute of Technology CambridgeMA United States CIFAR Azrieli Global Scholars program CIFAR Toronto Canada

The convergence of topology and correlations represents a highly coveted realm in the pursuit of novel quantum states of matter [1, 2]. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order [3- 10], not possible in quantum Hall and Chern insulator systems. However, the QSH insulator with quantized edge conductance remains rare, let alone that with significant correlations. In this work, we report a novel dual QSH insulator within the intrinsic monolayer crystal of TaIrTe4, arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe4 demonstrates the QSH insulator that aligns with single-particle band structure calculations, manifesting enhanced nonlocal transport and quantized helical edge conductance. Interestingly, upon introducing electrons from charge neutrality, TaIrTe4 only shows metallic behavior in a small range of charge densities but quickly goes into a new insulating state, entirely unexpected based on TaIrTe4's single-particle band structure. This insulating state could arise from a strong electronic instability near the van Hove singularities (VHS), likely leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state, marked by the revival of nonlocal transport and quantized helical edge conduction. Our observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands via CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism [3-5, 11, 12]. Copyright © 2024, The Authors. All rights reserved.

关键词： Charge density waves

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Correction: NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water

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New Journal of Chemistry 2023年第3期48卷 1443-1443页

作者： R. Robin Vinoth Kumar Raja R. Sathish Kumar G. Arthanareeswaran Wirach Taweepreda Membrane Research Laboratory Department of Chemical Engineering National Institute of Technology Tiruchirappalli 620015 India Department of Chemical Engineering National Institute of Technology Andhra Pradesh Tadepalligudem Andhra Pradesh 534101 India Polymers & Composites Lab Department of Biomaterials Saveetha Dental College and Hospitals Saveetha Institute of Medical and Technical Sciences Saveetha University Chennai 600077 India Polymer Science Program Division of Physical Science Faculty of Science Prince of Songkla University Hat-Yai Songkhla 90110 Thailand

Correction for ‘NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water’ by R. Robin et al., New J. Chem., 2023, 47, 20517–20526, https://***/10.1039/D3NJ03783E.

Correction for ‘NaCMC-decorated ZnO nanocomposite polymer membranes for the separation of reactive dyes from textile water’ by R. Robin et al., New J. Chem., 2023, 47, 20517–20526, https://***/10.1039/D3NJ03783E.

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Titelbild: Highly Dispersed Pd@ZIF-8 for Photo-Assisted Cross-Couplings and CO2to Methanol: Activity and Selectivity Insights (Angew. Chem. 48/2024)

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Angewandte Chemie 2024年第48期136卷

作者： Vijay K. Velisoju Enrique V. Ramos-Fernández Rajesh Kancherla Rafia Ahmad Kuntal Pal Hend Mohamed Jose L. Cerrillo Mark J. Meijerink Luigi Cavallo Magnus Rueping Pedro Castaño Multiscale Reaction Engineering KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia Laboratorio de Materiales Avanzados Departamento de Química Inorgánica—Instituto Universitario de Materiales de Alicante Universidad de Alicante Apartado 99 E-03080 Alicante Spain Chemical Engineering Program Physical Science and Engineering (PSE) Division KAUST Thuwal 23955-6900 Saudi Arabia

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Cover Picture: Highly Dispersed Pd@ZIF-8 for Photo-Assisted Cross-Couplings and CO2to Methanol: Activity and Selectivity Insights (Angew. Chem. Int. Ed. 48/2024)

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Angewandte Chemie International Edition 2024年第48期63卷

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Highly Dispersed Pd@ZIF-8 for Photo-Assisted Cross-Couplings and CO2to Methanol: Activity and Selectivity Insights

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Angewandte Chemie 2024年第48期136卷

Our study unveils a pioneering methodology that effectively distributes Pd species within a zeolitic imidazolate framework-8 (ZIF-8). We demonstrate that Pd can be encapsulated within ZIF-8 as atomically dispersed Pd species that function as an excited-state transition metal catalyst for promoting carbon–carbon (C−C) cross-couplings at room temperature using visible light as the driving force. Furthermore, the same material can be reduced at 250 °C, forming Pd metal nanoparticles encapsulated in ZIF-8. This catalyst shows high rates and selectivity for carbon dioxide hydrogenation to methanol under industrially relevant conditions (250 °C, 50 bar): 7.46 mol methanol mol metal −1 h −1 and >99 %. Our results demonstrate the correlations of the catalyst structure with the performances at experimental and theoretical levels.

关键词： Pd@ZIF-8 CO2 hydrogenation Alkyl halide Excited-state Palladium Cross-coupling

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Cavity-mediated superthermal phonon correlations in the ultrastrong coupling regime

arXiv

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arXiv 2024年

作者： Kim, Dasom Hou, Jin Lee, Geon Agrawal, Ayush Kim, Sunghwan Zhang, Hao Bao, Di Baydin, Andrey Wu, Wenjing Tay, Fuyang Huang, Shengxi Chia, Elbert E.M. Kim, Dai-Sik Seo, Minah Mohite, Aditya D. Hagenmüller, David Kono, Junichiro Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX77005 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States Sensor System Research Center Korea Institute of Science and Technology Seoul02792 Korea Republic of Department of Physics and Astronomy Seoul National University Seoul08826 Korea Republic of Department of Chemical and Biomolecular Engineering Rice University Houston77005 United States Ulsan44919 Korea Republic of Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore637371 Singapore Smalley–Curl Institute Rice University HoustonTX77005 United States Rice Advanced Materials Institute Rice University HoustonTX77005 United States KU–KIST Graduate School of Converging Science and Technology Korea University Seoul02841 Korea Republic of Université de Strasbourg CNRS Strasbourg67200 France Department of Physics and Astronomy Rice University HoustonTX77005 United States

Phonons, or vibrational quanta, are behind some of the most fundamental physical phenomena in solids, including superconductivity, Raman processes, and broken-symmetry phases. It is therefore of fundamental importance to find ways to harness phonons for controlling these phenomena and developing novel quantum technologies. However, the majority of current phonon control techniques rely on the use of intense external driving fields or strong anharmonicities, which restricts their range of applications. Here, we present a scheme for controlling the intensity fluctuations in phonon emission at room temperature based on multimode ultrastrong light–matter coupling. The multimode ultrastrong coupling regime is achieved by coupling two optical phonon modes in lead halide perovskites to an array of nanoslots, which operates as a single-mode cavity. The extremely small mode volume of the nanoslots enables unprecedented coupling strengths in a cavity phonon-polariton system. In the far-detuned, low-cavity-frequency regime, we demonstrate that the nanoslot resonator mediates an effective coupling between the phonon modes, resulting in superthermal phonon bunching in thermal equilibrium, both within the same mode and between different modes. Experimental results are in good agreement with a multimode Hopfield model. Our work paves the way for the tailoring of phonons to modify charge and energy transport in perovskite materials, with potential applications in light-collecting or emitting devices. Copyright © 2024, The Authors. All rights reserved.

关键词： Perovskite

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Nonreciprocal transport in a bilayer of MnBi2Te4 and Pt

arXiv

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arXiv 2022年

作者： Ye, Chen Xie, Xiangnan Lv, Wenxing Huang, Ke Yang, Allen Jian Jiang, Sicong Liu, Xue Zhu, Dapeng Qiu, Xuepeng Tong, Mingyu Zhou, Tong Hsu, Chuang-Han Chang, Guoqing Lin, Hsin Li, Peisen Yang, Kesong Wang, Zhenyu Jiang, Tian Wang, Xiao Renshaw Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 21 Nanyang Link 637371 Singapore State Key Laboratory of High Performance Computing College of Computer Science and Technology National University of Defense Technology Changsha410073 China Physics Laboratory Industrial Training Center Shenzhen Polytechnic Guangdong Shenzhen518055 China Department of NanoEngineering Program of Chemical Engineering University of California La Jolla San DiegoCA92093-0448 United States Program of Materials Science and Engineering University of California La Jolla San DiegoCA92093-0418 United States Institutes of Physical Science and Information Technology Anhui University Hefei230601 China Fert Beijing Institute MIIT Key Laboratory of Spintronics School of Integrated Circuit Science and Engineering Beihang University Beijing100191 China Beihang-Goertek Joint Microelectronics Institute Qingdao Research Institute Beihang University Qingdao266000 China Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology School of Physics Science and Engineering Tongji University Shanghai200092 China College of Advanced Interdisciplinary Studies National University of Defense Technology Changsha410073 China Insitute of Physics Academia Sinica Taipei115229 Taiwan College of Intelligence Science and Technology National University of Defense Technology Changsha410073 China National Innovation Institute of Defense Technology Academy of Military Sciences PLA China Beijing100010 China Beijing Academy of Quantum Information Sciences Beijing100084 China Beijing Institute for Advanced Study National University of Defense Technology Changsha410073 China School of Electrical and Electronic Engineering Nanyang Technological University 50 Nanyang Ave 639798 Singapore

MnBi2Te4 (MBT) is the first intrinsic magnetic topological insulator with the interaction of spin-momentum locked surface electrons and intrinsic magnetism, and it exhibits novel magnetic and topological phenomena. Recent studies suggested that the interaction of electrons and magnetism can be affected by the Mn-doped Bi2Te3 phase at the surface due to inevitable structural defects. Here we report an observation of nonreciprocal transport, i.e. current-direction-dependent resistance, in a bilayer composed of antiferromagnetic MBT and nonmagnetic Pt. The emergence of the nonreciprocal response below the Néel temperature confirms a correlation between nonreciprocity and intrinsic magnetism in the surface state of MBT. The angular dependence of the nonreciprocal transport indicates that nonreciprocal response originates from the asymmetry scattering of electrons at the surface of MBT mediated by magnon. Our work provides an insight into nonreciprocity arising from the correlation between magnetism and Dirac surface electrons in intrinsic magnetic topological insulators. © 2022, CC BY.

关键词： Magnetism

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Strong and Ultra-tough Ionic Hydrogel Based on Hyperbranched Macro-Cross-linker: Influence of Topological Structure on Properties

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Angewandte Chemie 2023年第42期135卷

作者： Yu Jiang Dezhi Zhan Meng Zhang Ying Zhu Huiqing Zhong Yangfei Wu Qinwen Tan Xinhua Dong Daohong Zhang Nikos Hadjichristidis Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education & Hubei Key Laboratory of Catalysis and Materials Science Hubei R&D Center of Hyperbranched Polymers Synthesis and Applications South-Central Minzu University Wuhan 430074 P. R. China Polymer Synthesis Laboratory Chemical Science Program KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Kingdom of Saudi Arabia

The application of hydrogels often suffers from their inherent limitation of poor mechanical properties. Here, a carboxyl-functionalized and acryloyl-terminated hyperbranched polycaprolactone (PCL) was synthesized and used as a macro-cross-linker to fabricate a super strong and ultra-tough ionic hydrogel. The terminal acryloyl groups of hyperbranched PCL are chemically incorporated into the network to form covalent cross-links, which contribute to robust networks. Meanwhile, the hydrophobic domains formed by the spontaneous aggregation of PCL chains and coordination bonds between Fe 3+ and COO − groups serve as dynamic non-covalent cross-links, which enhance the energy dissipation ability. Especially, the influence of the hyperbranched topological structure of PCL on hydrogel properties has been well investigated, exhibiting superior strengthening and toughening effects compared to the linear one. Moreover, the hyperbranched PCL cross-linker also endowed the ionic hydrogel with higher sensitivity than the linear one when used as a strain sensor. As a result, this well-designed ionic hydrogel possesses high mechanical strength, superior toughness, and well ionic conductivity, exhibiting potential applications in the field of flexible strain sensors.

关键词： Hydrogels Hyperbranched Cross-Linkers Polycaprolactone Strain Sensors Super Toughness

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