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Solvation Rule for Solid-Electrolyte Interphase Enabler in Lithium-Metal Batteries

Angewandte Chemie 2020年第41期132卷

作者： Su C.-C. He M. Shi J. Amine R. Zhang J. Amine K. Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Avenue Lemont IL 60439 United States Department of Chemical and Environmental Engineering University of California-Riverside Riverside CA 92521 United States Materials Science Division Argonne National Laboratory 9700 S. Cass Avenue Lemont IL 60439 United States Program of Materials Science and Engineering University of California-Riverside Riverside CA 92521 United States Material Science and Engineering Stanford University Stanford CA 94305 United States IRMC Imam Abdulrahman Bin Faisal University (IAU) Dammam 34212 Saudi Arabia

Despite the exceptionally high energy density of lithium metal anodes, the practical application of lithium-metal batteries (LMBs) is still impeded by the instability of the interphase between the lithium metal and the electrolyte. To formulate a functional electrolyte system that can stabilize the lithium-metal anode, the solvation behavior of the solvent molecules must be understood because the electrochemical properties of a solvent can be heavily influenced by its solvation status. We unambiguously demonstrated the solvation rule for the solid-electrolyte interphase (SEI) enabler in an electrolyte system. In this study, fluoroethylene carbonate was used as the SEI enabler due to its ability to form a robust SEI on the lithium metal surface, allowing relatively stable LMB cycling. The results revealed that the solvation number of fluoroethylene carbonate must be ≥1 to ensure the formation of a stable SEI in which the sacrificial reduction of the SEI enabler subsequently leads to the stable cycling of LMBs. © 2020 Wiley-VCH GmbH

关键词： anode stabilization electrolyte solvation lithium-metal batteries solid-electrolyte interphase solvation numbers

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Robust Coupling between Structural and Electronic Transitions in a Mott material

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Physical Review Letters 2019年第5期122卷 057601-057601页

作者： Yoav Kalcheim Nikita Butakov Nicolas M. Vargas Min-Han Lee Javier del Valle Juan Trastoy Pavel Salev Jon Schuller Ivan K. Schuller Department of Physics and Center for Advanced Nanoscience University of California San Diego La Jolla California 92093 USA Department of Electrical and Computer Engineering University of California Santa Barbara Santa Barbara California 93106 USA Material Science and Engineering Program University of California San Diego La Jolla California 92093 USA

The interdependences of different phase transitions in Mott materials are fundamental to the understanding of the mechanisms behind them. One of the most important relations is between the ubiquitous structural and electronic transitions. Using IR spectroscopy, optical reflectivity, and x-ray diffraction, we show that the metal-insulator transition is coupled to the structural phase transition in V2O3 films. This coupling persists even in films with widely varying transition temperatures and strains. Our findings are in contrast to recent experimental findings and theoretical predictions. Using V2O3 as a model system, we discuss the pitfalls in measurements of the electronic and structural states of Mott materials in general, calling for a critical examination of previous work in this field. Our findings also have important implications for the performance of Mott materials in next-generation neuromorphic computing technology.

关键词： Crystal growth Crystal orientation Crystal structure Crystal symmetry Crystallization Electronic structure Peierls transition Phase transitions Spin state transition Strain Antiferromagnets Mott insulators Stimuli-responsive materials Strongly correlated systems Thin films Cavity resonators Crystallography Fourier transform infrared spectroscopy Resistivity measurements Scanning techniques Sputtering Strain engineering X-ray diffraction

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Calculations of the Lu3N@C80 two-isomer equilibrium

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Fullerenes, Nanotubes & Carbon Nanostructures 2019年第5期27卷 382-386页

作者： Slanina, Zdeněk Uhlík, Filip Feng, Lai Akasaka, Takeshi Lu, Xing Adamowicz, Ludwik State Key Laboratory of Materials Processing and Die & Mould Technology School of Material Science and Engineering Huazhong University of Science and Technology Wuhan China Department of Physical and Macromolecular Chemistry Charles University Faculty of Science Praha 2 Czech Republic College of Physics Optoelectronics and Energy & Collaborative Innovation Center of Suzhou Nano Science and Technology Soochow University Suzhou China Department of Chemistry & Biochemistry University of Arizona Tucson AZ USA

Computations of the relative concentrations are reported for the two isomers of Lu3N@C80 experimentally known, i.e., produced by encapsulation into the isolated-pentagon-rule (IPR) C80 cages with Ih and symmetries. The calculations are mostly based on the density-functional theory (DFT) treatments with the B3LYP functional. The inter-isomeric energetics is further refined with the MP2 perturbation method which places the endohedral higher in the potential energy by 16.9 kcal/mol. The isomeric populations are evaluated using the Gibbs energy in a broad temperature interval. The computations performed with the floating-encapsulate-model (FEM) treatment can reasonably reproduce the observed isomeric ratio, thus pointing out a need for adequate representation of the dynamic endohedral symmetry. [ABSTRACT FROM AUTHOR]

关键词： Clusterfullerenes DFT and MP2 computations Gibbs-energy evaluations IPR fullerene cages isomeric populations Lu3N@C80 metallofullerenes

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Microscopic picture of paraelectric perovskites from structural prototypes

arXiv

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arXiv 2021年

作者： Kotiuga, Michele Halilov, Samed Kozinsky, Boris Fornari, Marco Marzari, Nicola Pizzi, Giovanni École Polytechnique Fédérale de Lausanne LausanneCH-1015 Switzerland Designed Material Technologies LLC P.O. Box 14548 RichmondVA23221-9998 United States John A. Paulson School of Engineering and Applied Sciences Harvard University 29 Oxford Street CambridgeMA02138 United States Robert Bosch LLC Research and Technology Center CambridgeMA02139 United States Department of Physics Science of Advanced Materials Program Central Michigan University Mt. PleasantMI48859 United States

We highlight with first-principles molecular dynamics the persistence of intrinsic h111i Ti off-centerings for BaTiO3 in its cubic paraelectric phase. Intriguingly, these are inconsistent with the Pm¯3m space group often used to atomistically model this phase using density functional theory or similar methods. Therefore we deploy a systematic symmetry analysis to construct representative structural models in the form of supercells that satisfy a desired point symmetry but are built from the combination of lower-symmetry primitive cells. We define as structural prototypes the smallest of these that are both energetically and dynamically stable. Remarkably, two 40-atom prototypes can be identified for paraelectric BaTiO3;these are also common to many other ABO3 perovskites. These prototypes can offer structural models of paraelectric phases that can be used for the computational engineering of functional materials. Last, we show that the emergence of B-cation off-centerings and the primitive-cell phonon instabilities is controlled by the equilibrium volume, in turn dictated by the filler A cation. © 2021, CC BY.

关键词： Positive ions

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Discovery of ionic impact ionization (I3) in perovskites triggered by a single photon

arXiv

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arXiv 2019年

作者： Xu, Zihan Yu, Yugang Niaz, Iftikhar Ahmad Chen, Yimu Arya, Shaurya Lei, Yusheng Miah, Mohammad Abu Raihan Zhou, Jiayun Zhang, Alex Ce Yan, Lujiang Xu, Sheng Nomura, Kenji Lo, Yu-Hwa Department of NanoEngineering University of California San DiegoCA United States Material Science and Engineering Program University of California San DiegoCA United States Department of Electrical and Computer Engineering University of California San DiegoCA United States

Organic-inorganic metal halide perovskite devices have generated significant interest for LED, photodetector, and solar cell applications due to their attractive optoelectronic properties and substrate-choice flexibility1-4. These devices exhibit slow time-scale response, which have been explained by point defect migration5-6. In this work, we report the discovery of a room temperature intrinsic amplification process in methylammonium lead iodide perovskite (MAPbI3) that can be triggered by few photons, down to a single photon. The electrical properties of the material, by way of photoresponse, are modified by an input energy as small as 0.19 attojoules, the energy of a single photon. These observations cannot be explained by photo-excited electronic band-to-band transitions or prevailing model of photoexcited point defect migration since none of the above can explain the observed macroscopic property change by absorption of single or few photons. The results suggest the existence of an avalanche-like collective motion of iodides and their accumulation near the anode, which we will call "ionic impact ionization" (I3 mechanism). The proposed I3 process is the ionic analog of the electronic impact ionization, and has been considered impossible before because conventionally it takes far more energy to move ions out of their equilibrium position than electrons. We have performed first principle calculations to show that in MAPbI3 the activation energy for the I3 mechanism is appreciably lower than the literature value of the activation energy for the electronic impact ionization. The discovery of I3 process in perovskite material opens up possibilities for new classes of devices for photonic and electronic applications. Copyright © 2019, The Authors. All rights reserved.

关键词： Iodine compounds

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Nonlinear Supramolecular Polymers for Therapeutic Applications (vol 2, 1800103, 2019)

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ADVANCED THERAPEUTICS 2019年第5期2卷

作者： Chen, Wenzhuo Kretzschmann, Annika Tian, Wei Wu, Si MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions Shanxi Key Laboratory of Macromolecular Science and Technology School of Science Northwestern Polytechnical University Xi'an China Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter Chemistry Anhui Key Laboratory of Optoelectronic Science and Technology Department of Polymer Science and Engineering University of Science and Technology of China Hefei China Max Planck Institute for Polymer Research Ackermannweg 10 Mainz Germany

An elegant combination of supramolecular polymers exhibiting nonlinear topological structures results in a series of brand new, nonlinear supramolecular polymers. Recently, these polymers have attracted increased attention in various fields due to their diverse and advantageous properties. Especially in therapeutic applications, one can take advantage of their unique chemical, physical, and biological properties such as degradability and stimuli-responsiveness. Due to the large number of possible module modifications, such polymers have great potential as platforms in disease treatments. In this review, the structures, properties, and functions of different nonlinear supramolecular polymers are summarized. Current therapeutic applications are presented and the prospective design trends are discussed for promoting the development of nonlinear supramolecular polymers.

关键词： drug delivery nanomedicine polymers supramolecules therapeutics

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Microstructural and Micro-Chemical Evolutions in Irradiated UCO Fuel Kernels of AGR-1 and AGR-2 TRISO Fuel Particles

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Journal of Physics: Conference Series 2021年第1期2048卷

作者： Zhenyu Fu Yong Yang Isabella J. Van Rooyen Subhashish Meher Boopathy Kombaiah Nuclear Engineering Program Department of Materials Science and Engineering University of Florida PO Box 116400 100 Rhines Hall Gainesville FL 32611 USA Fuel Design and Development Department Idaho National Laboratory Idaho Falls ID 83415-6188 USA Material Science Department Idaho National Laboratory Idaho Falls ID 83415-6188 USA Advanced Characterization Department Idaho National Laboratory Idaho Falls ID 83415-6188 USA

AGR-1 and AGR-2 tristructural-isotropic (TRISO) fuel particles were fabricated using slightly different fuel kernel chemical compositions, modified fabrication processes, different fuel kernel diameters, and changed 235U enrichments. Extensive microstructural and analytical characterizations were conducted to correlate those differences with the fuel kernels' responses to neutron irradiations in terms of irradiated fuel microstructure, fission products' chemical and physical states, and fission gas bubble evolutions. The studies used state-of-the-art transmission electron microscopy (TEM) equipped with energy-dispersive x-ray spectroscopy (EDS) via four silicon solid-state detectors with super sensitivity and rapid speed. The TEM specimens were prepared from selected AGR-1 and AGR-2 irradiated fuel kernels exposed to safety testing after irradiation. The particles were chosen in order to create representative irradiation conditions with fuel burnup in the range of 10.8 to 18.6% fissions per initial metal atom (FIMA) and time-average volume-average temperatures varying from 1070 to 1287°C. The 235U enrichment was 19.74 wt.% and 14.03 wt.% for the AGR-1 and AGR-2 fuel kernels, respectively. The TEM results showed significant microstructural reconstructions in the irradiated fuel kernels from both the AGR-1 and AGR-2 fuels. There are four major phases: fuel matrix of UO2 and UC, U2RuC2, and UMoC2—in the irradiated AGR-2 fuel kernel. Zr and Nd form a solid solution in the UC phase. The UMoC2 phase often features a detectable concentration of Tc. Pd was mainly found to be located in the buffer layer or associated with fission gas bubbles within the UMoC2 phase. EDS maps qualitatively show that rare-earth fission products (Nd et al.) preferentially reside in the UO2 phase. In contrast, in the irradiated AGR-1 fuel kernel, no U2RuC2 or UMoC2 precipitates were positively identified. Instead, there was a high number of rod-shaped precipitates enriched with Ru, Tc, Rh, and Pd

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Erratum: “Two-dimensional porous graphitic carbon nitride C6N7 monolayer: First-principles calculations” [Appl. Phys. Lett. 119, 142102 (2021)]

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Applied Physics Letters 2022年第18期120卷

作者： A. Bafekry M. Faraji M. M. Fadlallah I. Abdolhosseini Sarsari H. R. Jappor S. Fazeli M. Ghergherehchi 1Department of Radiation Application Shahid Beheshti University Tehran Iran 2Micro and Nanotechnology Graduate Program TOBB University of Economics and Technology Sogutozu Caddesi No 43 Sogutozu 06560 Ankara Turkey 3Department of Physics Faculty of Science Benha University 13518 Benha Egypt 4Department of Physics Isfahan University of Technology Isfahan 84156-83111 Iran 5Department of Physics College of Education for Pure Sciences University of Babylon Hilla Iraq 6Department of Material Science and Engineering Sharif University of Technology PO Box 11155-9466 Tehran Iran 7Department of Electrical and Computer Engineering Sungkyunkwan University 16419 Suwon South Korea

The original article1 contains misprints in the values of the elastic parameters. The values of C11 = 258.6 GPa, C22 = 290.8 GPa, and C12 = 70.73 GPa and C13 =

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Superior Metal-Organic Framework Activation with Dimethyl Ether

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Angewandte Chemie 2022年第52期134卷

作者： Keenan R. Wright Dr. Karabi Nath Prof. Dr. Adam J. Matzger Department of Chemistry Institution University of Michigan 930 North University Avenue Ann Arbor MI 48109-1055 USA Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Methodology (supporting) Writing - review & editing (supporting) Department of Chemistry and Macromolecular Science and Engineering Program University of Michigan 930 North University Avenue Ann Arbor MI 48109-1055 USA

Metal–organic frameworks (MOFs) are demonstrated to be readily activated by treatment with the low surface tension, low boiling point solvent dimethyl ether (DME). The mildness of the method enables access to high surface areas by avoiding structural changes in the framework that often plague thermal activation methods. A distinction from previous methods is that DME activation succeeds for materials with coordinatively unsaturated sites (CUS) and non-CUS MOFs as well. DME displaces solvent molecules occupying the pores of the MOF as well as those coordinated to metal centers; reducing evacuation temperature by using a coordinating, yet highly volatile guest enables low temperature activation with structural retention as demonstrated surface area measurements that match or exceed existing activation protocols.

关键词： Coordination Chemistry Metal–Organic Frameworks Microporous materials Structural Collapse Surface Area

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Activatable NIR-II Photothermal Lipid Nanoparticles for Improved Messenger RNA Delivery

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Angewandte Chemie 2023年第25期135卷

作者： Dr. Benhao Li Dr. Mengyao Zhao Weiping Lai Dr. Xuanbo Zhang Bowei Yang Prof. Xiaoyuan Chen Prof. Qianqian Ni Departments of Diagnostic Radiology Surgery Chemical and Biomolecular Engineering and Biomedical Engineering Yong Loo Lin School of Medicine and Faculty of Engineering National University of Singapore Singapore 119074 Singapore Nanomedicine Translational Research Program NUS Centre for Nanomedicine Yong Loo Lin School of Medicine National University of Singapore Singapore 117597 Singapore Contribution: Investigation (lead) Writing - original draft (lead) Contribution: Investigation (supporting) Department of Chemistry State Key Laboratory of Molecular Engineering of Polymers and iChem Shanghai Key Laboratory of Molecular Catalysis and Innovative Material Fudan University Shanghai 200433 China Clinical Imaging Research Centre Centre for Translational Medicine Yong Loo Lin School of Medicine National University of Singapore Singapore 117599 Singapore Institute of Molecular and Cell Biology Agency for Science Technology and Research (A*STAR) Singapore 138673 Singapore Contribution: Funding acquisition (equal) Supervision (equal) Writing - review & editing (equal)

Endosomal escape remains a central issue limiting the high protein expression of mRNA therapeutics. Here, we present second near-infrared (NIR-II) lipid nanoparticles (LNPs) containing pH activatable NIR-II dye conjugated lipid (Cy-lipid) for potentiating mRNA delivery efficiency via a s timulus-responsive p hotothermal-promoted e ndosomal e scape d elivery (SPEED) strategy. In acidic endosomal microenvironment, Cy-lipid is protonated and turns on NIR-II absorption for light-to-heat transduction mediated by 1064 nm laser irradiation. Then, the heat-promoted LNPs morphology change triggers rapid escape of NIR-II LNPs from the endosome, allowing about 3-fold enhancement of enhanced green fluorescent protein (eGFP) encoding mRNA translation capacity compared to the NIR-II light free group. In addition, the bioluminescence intensity induced by delivered luciferase encoding mRNA in the mouse liver region shows positive correlation with incremental radiation dose, indicating the validity of the SPEED strategy.

关键词： Endosomal Escape Lipid Nanoparticle Photothermal Effect Second Near-Infrared Window

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