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arXiv 2023年

作者： Fabris, Guilherme S.L. Ferrer, Mateus M. Sambrano, Julio R. Almeida, Cláudio R.R. Paskocimas, Carlos A. La Porta, Felipe A. Graduate Program in Materials Science and Engineering Technological Development Center Universidade Federal de Pelotas RS Pelotas96010-610 Brazil Modeling and Molecular Simulation Group São Paulo State University Bauru São Paulo17033-360 Brazil Department of Materials Engineering Federal University of Rio Grande do Norte RN Natal59078-970 Brazil Postgraduate Program in Science and Engineering of Materials Federal University of Rio Grande do Norte RN Natal59078-970 Brazil Federal University of Technology - Paraná Nanotechnology and Computational Chemistry Laboratory Avenida dos Pioneiros 3131 CEP PR Londrina86036-370 Brazil State University of Londrina Post-Graduation Program in Chemistry Rodovia Celso Garcia Cid 445 km 380 CEP PR Londrina86057-970 Brazil

Lanarkite is a mineral formed by a combination of lead, sulphur, and oxygen atoms arranged in the general chemical formula Pb2SO5 (PSO) that crystallises with monoclinic symmetry (belonging to the C2/m space group, No. 12). This mineral was first discovered in Lanarkshire, Scotland and was named after its location. PSO has a unique structure comprising alternating penta-coordinated lead [PbO5] and tetra-coordinated sulphur [SO4] clusters. This lanarkite-type structure has recently attracted significant scientific interest and has been the focus of the superconducting material research community. However, its chemistry needs to be explored further. This article presents a comprehensive investigation on the chemical bonding, electronic structure, and spectroscopic properties of the lanarkite-type PSO structure from a computational perspective. Thus, different functionals in the DFT (e.g., PBE, PBE0, PBESOL, PBESOL0, BLYP, WC1LYP37, and B3LYP) were assessed to accurately predict their fundamental properties. All the DFT calculations were performed using a triple-zeta valence plus polarisation basis set. Among all the DFT functionals tested in this study, PBE showed the best agreement with the experimental data available in the literature. Our results also reveal that the [PbO5] clusters are formed with three Pb–O bond lengths, with values of about 2.32, 2.59, and 2.84 Å, respectively, while the [SO4] clusters have the same S–O bond length of 1.57 Å. We performed a complete topological analysis of this system to comprehend these structural differences. Additionally, the PSO structure has an indirect band gap energy of 2.9 eV and an effective mass ratio (mℎ∗ /me∗) of about 0.415 (using PBE calculations) which may, in principle, indicate a low recombination of electron-hole pairs in the lanarkite structure. Therefore, we believe that a detailed understanding of their electronic structures, spectroscopic properties as well as their chemical bonding is critically important

关键词： Lead compounds

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Continuous-flow photochemistry: An expanding horizon of sustainable technology

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Chinese chemical Letters 2020年第9期31卷 2395-2400页

作者： Jingli Xie Dongyuan Zhao College of Biological Chemical Science and EngineeringJiaxing UniversityJiaxing 314001China Chemistry and Chemical Engineering Guangdong Laboratory Guangdong Technion–Israel Institute of Technology(GTIIT)Shantou 515031China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Department of Chemistry and Laboratory of Advanced Materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersFudan UniversityShanghai 200433China

Understanding the unique characteristics of continuous-flow photochemistry will lead to a paradigm shift in the way we enhance sustainability and *** this mini-review,we first provide a succinct overview of working principles of this technique and discuss several recent synthetic ***,emphasis is given to those representative examples which address environmental issues such as indoor air pollutants and water ***,recent progress made using this technique to deal with rising CO2 emission,solar energy utilization and biomedical equipment is *** is believed that this mini-review could inspire more chemists to utilize this technique in their research,either in the academic or industrial field.

关键词： Continuous-flow photochemistry Synthesis Environmental application Micro-reaction technology Sustainable technology

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Van der Waals device integration beyond the limits of van der Waals forces via adhesive matrix transfer

arXiv

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arXiv 2023年

作者： Satterthwaite, Peter F. Zhu, Weikun Jastrzebska-Perfect, Patricia Tang, Melbourne Gao, Hongze Kitadai, Hikari Lu, Ang-Yu Tan, Qishuo Tang, Shin-Yi Chueh, Yu-Lun Kuo, Chia-Nung Lue, Chin Shan Kong, Jing Ling, Xi Niroui, Farnaz Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology CambridgeMA02139 United States Department of Chemical Engineering Massachusetts Institute of Technology CambridgeMA02139 United States Department of Chemistry Boston University BostonMA02215 United States Department of Materials Science and Engineering National Tsing Hua University Hsinchu30013 Taiwan Semiconductor Research Center Hon Hai Research Institute Taipei11492 Taiwan College of Semiconductor Research National Tsing Hua University Hsinchu30013 Taiwan Department of Physics National Cheng Kung University Tainan70101 Taiwan Taiwan Consortium of Emergent Crystalline Materials National Science and Technology Council Taipei10601 Taiwan Program on Key Materials Academy of Innovative Semiconductor and Sustainable Manufacturing National Cheng Kung University Tainan70101 Taiwan Division of Materials Science and Engineering Boston University BostonMA02215 United States The Photonics Center Boston University BostonMA02215 United States

Pristine van der Waals (vdW) interfaces between two-dimensional (2D) and other materials are core to emerging optical and electronic devices. Their direct fabrication is, however, challenged as the vdW forces are weak and cannot be tuned to accommodate integration of arbitrary layers without solvents, sacrificial-layers or high-temperatures, steps that can introduce damage. To address these limitations, we introduce a single-step 2D material-to-device integration approach in which forces promoting transfer are decoupled from the vdW forces at the interface of interest. We use this adhesive matrix transfer to demonstrate conventionally-forbidden direct integration of diverse 2D materials (MoS2, WSe2, PtS2, GaS) with dielectrics (SiO2, Al2O3), and scalable, aligned heterostructure formation, both foundational to device development. We then demonstrate a single-step integration of monolayer-MoS2 into arrays of transistors. With no exposure to polymers or solvents, clean interfaces and pristine surfaces are preserved, which can be further engineered to demonstrate both n- and p-type behavior. Beyond serving as a platform to probe the intrinsic properties of sensitive nanomaterials without the influence of processing steps, our technique allows efficient formation of unconventional device form-factors, with an example of flexible transistors demonstrated. Copyright © 2023, The Authors. All rights reserved.

关键词： Van der Waals forces

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Synergistic enhancement of lithium storage capacity in coal-based onion-like fullerenes by acidic oxidation pretreatment and chemical activation

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Journal of Energy Storage 2025年 129卷

作者： Ma, Xiao Yang, Weipeng Qin, Lei Wang, Ya Zhang, Wanggang Li, Yong Yang, Yongzhen Yan, Lingpeng Su, Qingmei Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education Taiyuan University of Technology Taiyuan 030024 China College of Materials Science and Engineering Taiyuan University of Technology Taiyuan 030024 China Department of Materials Science and Engineering Jinzhong University Shanxi Jinzhong 030619 China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030032 China Materials Institute of Atomic and Molecular Science Shaanxi University of Science and Technology Xi’ an 710021 China

Onion-like fullerenes (OLFs), with their high specific surface area, exceptional electrical conductivity, stable cycling performance, and tunable electrochemical characteristics, have shown great potential as anode materials in enhancing energy density, power density, and cycle life of energy storage batteries. In this study, anthracite coal is employed as the precursor to efficiently prepare coal-based OLFs (C-OLFs) via the one-step thermocatalytic method. To improve their lithium storage performance, acid oxidation treatment of precursor and chemical activation treatment of product are employed. The effects of these two treatments on the morphology, structure, and electrochemical properties of the C-OLFs are systematically investigated. The results indicate that the one-step thermocatalytic method enables rapid preparation of C-OLFs at the temperature of 1600 °C. The C-OLFs obtained through nitric acid oxidation of coal exhibits a higher degree of graphitization compared with those treated through mixed acid oxidation of coal. C-OLFs prepared by nitric acid oxidation of coal at 80 °C exhibits the highest degree of graphitization, with a Coulombic efficiency of up to 80 %. While C-OLFs derived from coal oxidized at 120 °C demonstrates the optimal rate capability, maintaining a lithium storage specific capacity of 140 mAh·g⁻¹, even at the high current density of 5 A·g⁻¹. Further chemical activation treatment of C-OLFs significantly enhances their lithium storage specific capacity, reaching 298 and 454 mAh·g⁻¹ for the initial and 100th cycles, respectively. This work provides fundamental data and experimental supports for the preparation of coal-based OLFs as anode materials for lithium-ion batteries.

关键词： Anthracite Graphitization Lithium-ion batteries Onion-like fullerenes Thermocatalytic

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Optical and spin coherence of Er3+ in epitaxial CeO2 on silicon

arXiv

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arXiv 2023年

作者： Zhang, Jiefei Grant, Gregory D. Masiulionis, Ignas Solomon, Michael T. Bindra, Jasleen K. Niklas, Jens Dibos, Alan M. Poluektov, Oleg G. Heremans, F. Joseph Guha, Supratik Awschalom, David D. Materials Science Division Argonne National Laboratory LemontIL60439 United States Center for Molecular Engineering Argonne National Laboratory LemontIL60439 United States Pritzker School of Molecular Engineering University of Chicago ChicagoIL60637 United States Chemical Sciences and Engineering Division Argonne National Laboratory LemontIL60439 United States Nanoscience and Technology Division Argonne National Laboratory LemontIL60439 United States Center for Nanoscale Materials Argonne National Laboratory LemontIL60439 United States Department of Physics University of Chicago ChicagoIL60637 United States

Solid-state atomic defects with optical transitions in the telecommunication bands, potentially in a nuclear spin free environment, are important for applications in fiber-based quantum networks. Erbium ions doped in CeO2 offer such a desired combination. Here we report on the optical homogeneous linewidth and electron spin coherence of Er3+ ions doped in CeO2 epitaxial film grown on a Si(111) substrate. The long-lived optical transition near 1530 nm in the environmentally-protected 4f shell of Er3+ shows a narrow homogeneous linewidth of 440 kHz with an optical coherence time of 0.72 µs at 3.6 K. The reduced nuclear spin noise in the host allows for Er3+ electron spin polarization at 3.6 K, yielding an electron spin coherence of 0.66 µs (in the isolated ion limit) and a spin relaxation of 2.5 ms. These findings indicate the potential of Er3+:CeO2 film as a valuable platform for quantum networks and communication applications. © 2023, CC BY-NC-SA.

关键词： Cerium oxide

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Role of the Ionomer in Supporting Electrolyte-Fed Anion Exchange Membrane Water Electrolyzers

ACS electrochemistry

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ACS electrochemistry 2025年第2期1卷 239-248页

作者： Emily K Volk Arielle L Clauser Melissa E Kreider Diego D Soetrisno Sunilkumar Khandavalli Joshua D Sugar Stephanie Kwon Shaun M Alia Advanced Energy Systems Graduate Program Colorado School of Mines Golden Colorado 80401 United States. Sandia National Laboratories Livermore California 94550 United States. Chemistry and Nanoscience Center National Renewable Energy Laboratory Golden Colorado 80401 United States. Materials Science Center National Renewable Energy Laboratory Golden Colorado 80401 United States. Department of Chemical and Biological Engineering Colorado School of Mines Golden Colorado 80401 United States.

While anion exchange membrane water electrolyzers (AEMWEs) have achieved significant performance advances in recent decades, overpotentials remain high relative to their proton exchange membrane water electrolyzer (PEMWE) counterparts, requiring AEMWE-specific catalyst layer design strategies to further advance this technology. In this work, the role of the ionomer in catalyst layer structure and quality, catalyst layer stability, and ion conduction for supporting electrolyte-fed AEMWEs is assessed for catalyst layers composed of NiFeO and PiperION TP85 from Versogen at variable ionomer contents (0-30 wt %) for tests up to 200 h. The results reveal that, for supporting electrolyte-fed AEM devices, the ionomer is not required for ion conduction through the catalyst layer. Instead, the ionomer is found to play a critical role in catalyst layer structure and stability, where intermediate ionomer contents lead to the lowest overpotentials, highest effective surface areas, and lowest catalyst layer resistances. Catalyst layer stability is found to be a function of both catalyst adhesion and ionomer loss. These results show that an ionomer may be selected which is not of the same chemistry as the anion exchange membrane, mitigating ionomer stability concerns throughout the catalyst layer and offering a pathway towards highly active and stable AEMWEs.

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Metal ratio and bimetal nanoarchitectonics of ammonia-based fluoride complex induced nickel hydroxide and manganese oxide composites as active materials of an energy storage device

引用

Journal of Energy Storage 2024年 80卷

作者： Hsu, Chuan-Chih Yu, You Zher Wu, Chung-Hsien Lee, Pin-Yan Chen, Hung-Ming Husain, Sadang Kongvarhodom, Chutima Hsiao, Yu-Cheng Lin, Lu-Yin Division of Cardiovascular Surgery Department of Surgery School of Medicine College of Medicine Taipei Medical University Taiwan Division of Cardiovascular Surgery Department of Surgery Taipei Medical University Hospital Taiwan Department of Chemical Engineering and Biotechnology National Taipei University of Technology Taipei Taiwan Gingen Technology Co. LTD. Rm. 7 10F. No.189 Sec. 2 Keelung Rd. Xinyi Dist. Taipei11054 Taiwan Department of Physics Faculty of Mathematics and Natural Science Lambung Mangkurat University Banjarmasin70124 Indonesia Department of Chemical Engineering King Mongkut's University of Technology Thonburi 126 Pracha-u-thit Toong-kru Bangkok10140 Thailand Department of Chemical Engineering Ming Chi University of Technology New Taipei City24301 Taiwan Cell Physiology and Molecular Image Research Center Wan Fang Hospital Taipei Medical University Taipei11696 Taiwan International PhD Program in Biomedical Engineering College of Biomedical Engineering Taipei Medical University Taipei11031 Taiwan Stanford Byers Center for Biodesign Stanford University CA94305-5428 United States Graduate Institute of Biomedical Optomechatronics College of Biomedical Engineering Taipei Medical University Taipei11031 Taiwan

Nickel and manganese compounds are widely applied as efficient battery-type active materials for energy storage devices, due to high theoretical capacities and abundant redox states for generating redox reactions to store charges. Morphology plays significant roles on energy storage ability. Structure directing agent (SDA) is widely reported to have ability for modulating configurations of active materials and to achieve excellent surface properties. In this work, it is the first time to use NH4BF4 and NH4HF2 as structure directing agents for synthesizing nickel manganese compounds derived from ZIF67 as active materials of energy storage devices. Bimetallic compounds are composed of nickel hydroxide and manganese oxide, which presents the favorable two-dimensional flower-like structure with high surface area and abundant redox states. The largest specific capacitance (CF) of 1358.2 F/g corresponding to the capacity of 226.4 mAh/g are achieved for the bimetallic compound synthesized using the Ni to Mn precursor ratio of 1 to 1 (NiMn11). The energy storage device assembled using NiMn11 and reduced graphene oxide on Ni foams presents a maximum energy density of 11.45 Wh/kg at the power density of 0.35 kW/kg, and excellent long-term stability with the CF retention of 85.6% and Coulombic efficiency of 87.5% after 10,000 cycles. © 2023

关键词： Fluorine compounds

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Shape Anisotropy-Governed High-Performance Nanomagnetosol for In Vivo Magnetic Particle Imaging of Lungs

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Small 2024年第5期20卷 e2305300页

作者： Nigam, Saumya Mohapatra, Jeotikanta Makela, Ashley V. Hayat, Hanaan Rodriguez, Jessi Mercedes Sun, Aixia Kenyon, Elizabeth Redman, Nathan A. Spence, Dana Jabin, George Gu, Bin Ashry, Mohamed Sempere, Lorenzo F. Mitra, Arijit Li, Jinxing Chen, Jiahui Wei, Guo-Wei Bolin, Steven Etchebarne, Brett Liu, J. Ping Contag, Christopher H. Wang, Ping Precision Health Program Michigan State University East LansingMI48824 United States Department of Radiology College of Human Medicine Michigan State University East LansingMI48824 United States Department of Physics The University of Texas at Arlington ArlingtonTX76019 United States Michigan State University East LansingMI48824 United States Department of Biomedical Engineering College of Engineering Michigan State University East LansingMI48824 United States Human Biology Program College of Natural Science Michigan State University East LansingMI48824 United States Department of Obstetrics Gynecology and Reproductive Sciences College of Human Medicine Michigan State University East LansingMI48824 United States Department of Materials Science and Engineering National Cheng Kung University Tainan City701 Taiwan Department of Mathematics College of Natural Science Michigan State U niversity East LansingMI48824 United States Department of Electrical and Computer Engineering College of Engineering Michigan State University East LansingMI48824 United States Department of Biochemistry and Molecular Biology College of Natural Science Michigan State University East LansingMI48824 United States Department of Pathobiology and Diagnostic Investigation College of Veterinary Medicine Michigan State University East LansingMI48824 United States Osteopathic Medical Specialties College of Osteopathic Medicine Michigan State University East LansingMI48824 United States Department of Microbiology and Molecular Genetics Michigan State University East LansingMI48824 United States

Caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), coronavirus disease 2019 (COVID-19) has shown extensive lung manifestations in vulnerable individuals, putting lung imaging and monitoring at the forefront of early detection and treatment. Magnetic particle imaging (MPI) is an imaging modality, which can bring excellent contrast, sensitivity, and signal-to-noise ratios to lung imaging for the development of new theranostic approaches for respiratory diseases. Advances in MPI tracers would offer additional improvements and increase the potential for clinical translation of MPI. Here, a high-performance nanotracer based on shape anisotropy of magnetic nanoparticles is developed and its use in MPI imaging of the lung is demonstrated. Shape anisotropy proves to be a critical parameter for increasing signal intensity and resolution and exceeding those properties of conventional spherical nanoparticles. The 0D nanoparticles exhibit a 2-fold increase, while the 1D nanorods have a > 5-fold increase in signal intensity when compared to VivoTrax. Newly designed 1D nanorods displayed high signal intensities and excellent resolution in lung images. A spatiotemporal lung imaging study in mice revealed that this tracer offers new opportunities for monitoring disease and guiding intervention. © 2023 The Authors. Small published by Wiley-VCH GmbH.

关键词： Nanorods

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Efficient removal for multiple pollutants via Ag_(2)O/BiOBr heterojunction:A promoted photocatalytic process by valid electron transfer pathway

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Chinese chemical Letters 2020年第10期31卷 2698-2704页

作者： Zhiruo Zhou Yanan Li Mingmei Li Yi Li Sihui Zhan College of Environmental Science and Engineering Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300071China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China Tianjin Key Lab for Rare Earth Materials and Applications Tianjin 300072China

Multiple pollutants including pathogenic microorganism contaminations and emerging organic contaminations(EOCs)have shown a growing threat to the environment,especially the natural ***,the control and removal of pathogenic microorganism contaminations and EOCs have been greatly limited since limited knowledge of their environmental ***,a novel and efficient photocatalyst Ag_(2)O/BiOBr heterojunction was synthesized and used for removal of multiple pollutants including Escherichia coli(***),Staphylococcus aureus(***),tetracycline and acetaminophen under visible *** results showed that there were valid electron transfer pathways between BiOBr and Ag_(2)O,the main electron transfer direction was the BiOBr to Ag_(2)***-generated electrons were stored in Ag_(2)O and thus separation efficiency between holes and photo-generated electrons was obviously *** oxygen species were highly produced and eventually end up with the high efficiency of removal of multiple *** Ag_(2)O/BiOBr with Ag_(2)O content at 3%(the best performance)under visible light,log decrease of *** was 7.16(removal efficiency was 100%)in 120 min,log decrease of *** was 7.23(removal efficiency was 100%)in 160 min,C/C0 of tetracycline was 0.06 in 180 min,C/C0 of acetaminophen was 0.17 in 180 *** work could provide a promising candidate in the actual contaminated natural waters for cleaning multiple pollutants.

关键词： Water pollution Photocatalysis Multiple pollutants Electrons transfer channels

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Effect of dual modification on structural, functional and dielectric properties of cassava starch

Food Physics

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Food Physics 2025年 2卷

作者： Cremasco, Paula Figueiredo M. Siqueira, Karine Mayuri Pistoni Sobral, Paulo José do Amaral Velloso, Walter Ferreira de Lima, César Gonçalves Gut, Jorge Andrey Wilhelms Moraes, Izabel Cristina Freitas Postgraduate Program in Materials Science and Engineering Faculty of Animal Science and Food Engineering University of São Paulo Avenue Duque de Caxias Norte São Paulo Pirassununga 13635900 Brazil Department of Biossistems Engineering Faculty of Animal Science and Food Engineering University of São Paulo Avenue Duque de Caxias Norte São Paulo Pirassununga 13635900 Brazil Department of Food Engineering Faculty of Animal Science and Food Engineering University of São Paulo Avenue Duque de Caxias Norte São Paulo Pirassununga 13635900 Brazil Food Research Center (FoRC) University of São Paulo Lake Street São Paulo São Paulo 05508-080 Brazil Departament of Basic Sciences Faculty of Animal Science and Food Engineering University of São Paulo Avenue Duque de Caxias Norte São Paulo Pirassununga 13635900 Brazil Department of Chemical Engineering Polytechnic School University of São Paulo Lake Street São Paulo São Paulo 05508-080 Brazil

The combined effect of hydrocolloid addition and microwave heating on the structural, physical and functional properties of cassava starch remains underexplored, despite individual studies on these modification methods. The dielectric properties, important for the microwave treatment of starch, have received little attention in recent studies. Cassava starch with and without addition of hydrocolloids (guar and xanthan gums) was modified by microwave heating for two different exposure times, and its structural, functional, and dielectric properties were studied. The dual modification enhanced the swelling power and oil holding capacity of the starch, reduced its gelatinization temperature, and did not alter its crystallinity. Notably, xanthan-modified starch microwaved for 6 min exhibited higher color variation (ΔE*) and increased granules agglomeration, while the microwave treatment alone roughened the surface of the starch granules. The mean diameters D[4,3] of starch increased with xanthan gum addition, microwave treatment (6 min), and their combination. The relative permittivity (ε’), loss factor (ε”) and penetration depth (D_p) were lower for samples modified by the combined method. Considering the type of hydrocolloid and the microwave exposure time, the combined modification significantly influenced the properties of starch, offering a promising approach to producing starch with enhanced functional properties. © 2024 KeAi Communications Co., Ltd

关键词： Biopolymers Cassava starch Guar Microwave Xanthan

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