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Deciphering the Impact of Polysulfide Solvation Structure on Electrical Double Layer Chemistry in Sodium–Sulfur Batteries

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Angewandte Chemie 2025年

作者： Weiqi Yao Min-Hao Pai Arumugam Manthiram Materials Science and Engineering Program & Walker Department of Mechanical Engineering The University of Texas at Austin Austin Texas 78712 USA

Room-temperature sodium–sulfur (RT Na–S) batteries are garnering attention for large-scale energy storage. However, their practical application is hindered by challenges, such as the shuttle effect of sodium polysulfides (NaPS) and dendrite growth. The high solubility of NaPS in the electrolyte is particularly problematic. It disrupts electron transfer and obstructs mass transport in the electrical double layer (EDL) region. The EDL plays a pivotal role in governing the interfacial chemistry between the electrode and electrolyte, significantly impacting the overall electrochemical performance. Through simulations and experimental screening of various solvents, including 1,2-dimethoxyethane (DME), tetrahydrofuran (THF), and tetrahydropyran (THP), along with ethyl 1,1,2,2-tetrafluoroethyl ether (ETFE) as a diluent, the relationship between NaPS solvation structure and EDL chemistry has been elucidated. Our findings reveal that THP-based localized high-concentration electrolyte (LHCE) not only reduces the solubility of NaPS by altering its solvation structure but also promotes the formation of a stable inorganic solid-electrolyte interphase (SEI) and improves compatibility with sodium metal. Consequently, Na–S batteries with LHCE-THP/ETFE exhibit long-term stability over 500 cycles at 1C rate with a capacity decay rate of only 0.07% per cycle. This study provides a methodology for designing electrolytes based on molecular structure, polysulfide solvation properties, and EDL interfacial chemistry.

关键词： Electrical double layer Electrolytes Polysulfide solvation structure Shuttle effect Sodium–sulfur batteries

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Coupling between bulk thermal defects and surface segregation dynamics

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Physical Review B 2021年第8期104卷 085408-085408页

作者： Jonathan Li Siming Zhang Chaoran Li Yaguang Zhu Jorge Anibal Boscoboinik Xiao Tong Jerzy T. Sadowski Guofeng Wang Guangwen Zhou Department of Mechanical Engineering & Materials Science and Engineering Program State University of New York Binghamton New York 13902 USA Department of Mechanical Engineering and Materials Science University of Pittsburgh Pittsburgh Pennsylvania 15261 USA Center for Functional Nanomaterials Brookhaven National Laboratory Upton New York 11973 USA

Surface segregation is a phenomenon that depends on the delicate interplay between thermodynamic driving forces and kinetic obstacles, for which elevated temperature is often needed to enhance the atom mobility and reach equilibrium. Using the classic system of Cu3Au(100) under nonisothermal conditions, herein, we show an adatom process underlying transient surface segregation dynamics through the temperature-change-driven creation and annihilation of thermal vacancies in the bulk and the resulting bulk-surface mass exchanges. This is demonstrated by monitoring the surface composition evolution of Cu3Au(100) with temperature changes between 250 and 500∘C, showing that the increase in temperature decreases monotonically the surface Au concentration as a result of the transfer of more Cu than Au from the bulk to the surface to form Cu-rich clusters of adatoms. Such a bulk thermal defect effect is expected to be universal in inducing the disparity in the bulk-surface mass exchanges of dissimilar atoms in multicomponent materials because of the inherent differences in the vacancy formation energies of the constituent atoms.

关键词： Self-diffusion Surface & interfacial phenomena Transition metal alloys Density functional calculations Ion beam analysis Mass spectrometry Scanning tunneling microscopy X-ray photoelectron spectroscopy

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Introducing self-healing properties to polyethersulfone (PES) membrane via poly(vinyl alcohol)/ polyacrylic acid (PVA/PAA) surface coating

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Chemosphere 2024年 349卷 140772页

作者： Lim, Yi Heng Wong, Eng Cheong Chong, Woon Chan Mohammad, Abdul Wahab Koo, Chai Hoon Lau, Woei Jye Department of Chemical Engineering Lee Kong Chian Faculty of Engineering and Science Universiti Tunku Abdul Rahman Sungai Long Campus Jalan Sungai Long Cheras Selangor Kajang43000 Malaysia Centre for Advanced and Sustainable Materials Research Universiti Tunku Abdul Rahman Sungai Long Campus Jalan Sungai Long Cheras Selangor Kajang43000 Malaysia Chemical and Water Desalination Program College of Engineering University of Sharjah Sharjah27272 United Arab Emirates Chemical Engineering Programme Faculty of Engineering and Built Environment Universiti Kebangsaan Malaysia Selangor Bangi43600 Malaysia Faculty of Chemical and Energy Engineering Universiti Teknologi Malaysia Johor Johor Bahru81310 Malaysia

During membrane filtration, it is inevitable that a membrane will experience physical damage, leading to a loss of its integrity and a decrease in separation efficiency. Hence, the development of a water-responsive membrane capable of healing itself autonomously after physical damage is significantly important in the field of water filtration. Herein, a water-enabled self-healing composite polyethersulfone (PES) membrane was synthesized by coating the membrane surface using a mixed solution composed of poly (vinyl alcohol) and polyacrylic acid (PVA-PAA). The self-healing efficiency of the coated PES membrane was examined based on the changes in water flux at three stages which are pre-damaged, post-damaged, and post-healing. The self-healing process was initiated by the swelling of the water-responsive PVA and PAA, followed by the formation of reversible hydrogen bonds, completing the self-healing process. The coated PES membrane with three layers of PVA-PAA coatings (at 3:1 ratio) demonstrated high water flux and remarkable self-healing efficiency of up to 98.3%. The self-healing capability was evidenced by the morphology of the membrane observed via scanning electron microscope (SEM). The findings of this investigation present a novel architecture approach for fabricating self-healing membranes using PVA-PAA, in addition to other relevant parameters as reported. © 2023 Elsevier Ltd

关键词： Membranes

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Influence of Temperature and Stress State on the Twip Behavior of 201ln and 316lv Austenitic Stainless Steels

SSRN

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SSRN 2022年

作者： Braga, Diogo Pedrino Corrêa, Leonardo Muthi Sordi, Vitor Luiz Rovere, Carlos Alberto Della Cintho, Osvaldo Mitsuyuki Kliauga, Andrea Madeira Federal University of São Carlos Graduate Program in Materials Science and Engineering São Carlos São Paulo Brazil Federal University of São Carlos Graduate Program in Mechanical Engineering São Carlos São Paulo Brazil Federal University of São Carlos Department of Materials Engineering São Carlos São Paulo Brazil State University of Ponta Grossa Department of Materials Engineering Ponta Grossa Paraná Brazil

The present results analyzed deformation behavior under tension and compression of two different austenitic stainless steels: AISI 201LN, with low nickel content and stabilized with Mn and N;and AISI 316LV, stabilized with Ni and with low content of interstitial atoms. Mechanical tests were performed at 10 -3 s -1 and at temperatures varying from -100 to 600 o C to yield comparable values of the stacking fault energy (SFE). The resulting microstructure was analyzed by X-ray diffraction and EBSD. The stress-strain curves were analyzed using the Kocks-Mecking (K-M) approach. For comparable stacking fault energies, temperature enhances the thermal activation effects that led to lower fraction of mechanical twins in the 201LN compared with the 316LV. The crystallographic re-orientation followed the flow rule irrespective of the temperature and deformation mechanism: tension and compression experiments showed the or orientation with the tension axis, respectively. In tension the dislocation storage and recovery factors of the K-M model were larger than in the compression and the amount of stored dislocations and crystallite size reflect these effects. In the compression, the TWIP effect was reduced for the 316LV and suppressed for the 201LN. © 2022, The Authors. All rights reserved.

关键词： Stacking faults

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Enhanced Cuproptosis via Metabolic Reprogramming Using Copper-Delivering Co-N-C Single-Atom Nanozyme

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ACS nano 2025年第24期19卷 2025 Jun 11页

作者： Kang Kim Jaewoo Lee Ok Kyu Park Hyochul Lee Taekyu Jang Jungho Kim Bowon Lee Jeong Hyun Kim Jaeho Moon Seoin Back Nohyun Lee Seung Hong Choi Taeghwan Hyeon Center for Nanoparticle Research Institute for Basic Science (IBS) Seoul 08826 Republic of Korea. School of Chemical and Biological Engineering and Institute of Chemical Processes Seoul National University Seoul 08826 Republic of Korea. Department of Radiology Seoul National University College of Medicine Seoul 03080 Republic of Korea. Interdisciplinary Program in Cancer Biology Seoul National University College of Medicine Seoul 03080 Republic of Korea. Department of Chemical and Biomolecular Engineering Sogang University Seoul 04107 Republic of Korea. KU-KIST Graduate School of Converging Science and Technology Korea University Seoul 02841 Republic of Korea. Department of Integrative Energy Engineering Korea University Seoul 02841 Republic of Korea. School of Advanced Materials Engineering Kookmin University Seoul 02707 Republic of Korea.

Cuproptosis, a copper-dependent cell death, has shown promise as a cancer therapy characterized by mitochondrial protein aggregation. However, this distinct feature makes its efficacy highly dependent on the metabolic state of cancer cells, yielding poor outcomes in hypoxic tumors with a reduced mitochondrial activity. Herein, we construct a Cu-delivering vehicle with catalase-like activity using oxygen-rich cobalt single-atom nanozymes (Cu@CoNC(O)) to reprogram metabolism while delivering copper. By introduction of oxygen-containing functional groups onto carbon supports, Cu@CoNC(O) exhibits significantly improved loading efficiency of Cu ions compared to its oxygen-deficient counterpart. Simultaneously, the outstanding catalase-like activity of Cu@CoNC(O) alleviates hypoxia, switching metabolism from glycolysis to mitochondrial respiration through the inhibition of lactate metabolism and activation of the pyruvate dehydrogenase complex. The synergistic effect of the metabolic shift and efficient Cu delivery promotes cuproptosis even under hypoxic conditions, leading to enhanced therapeutic effects. This study demonstrates the potential of single-atom nanozymes as catalytic ion delivery vehicles capable of concurrently performing catalytic functions and delivering metal ions, presenting an effective strategy to enhance cuproptosis through metabolic modulation.

关键词： catalase-like activity cuproptosis hypoxia relief ion delivery metabolic reprogramming single-atom nanozymes

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Halide Double Perovskite-Based Efficient Mechanical Energy Harvester and Storage Devices for Self-Charging Power Unit

SSRN

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SSRN 2022年

作者： Yoon, Soon-Gil Ippili, Swathi Kim, Jong Heon Jella, Venkatraju Behera, Subhashree Vuong, Van-Hoang Jung, Jang-Su Cho, Yujang Ahn, Jaewan Kim, Il-Doo Chang, Yun Hee Kim, Hyun-Suk Department of Materials Science and Engineering Chungnam National University 99 Daehak-ro Yuseong-gu Daejeon34134 Korea Republic of Texas Materials Institute and Materials Science and Engineering Program The University of Texas AustinTX78712 United States 291 Daehak-ro Yuseong-gu Daejeon34141 Korea Republic of

With the rapid development of portable/wearable electronic devices, high-efficient and sustainable self-powered systems have considerably risen in demand to support their off-grid operation. Recently, metal halide perovskites (MHPs) have been suggested as promising materials for energy harvesting and storage devices because of their excellent optoelectronic, ferro/piezoelectric, and ion migration properties. However, the high toxicity and poor physicochemical stability of MHPs obstruct their practical application. Herein, for the first time, the potential of methylammonium tin halide (MA2SnX6;X = Cl, Br, and I) double perovskite thin films for high-efficient self-charging power units (SPUs) is elucidated by virtue of their high stability in air. To this end, the integration of a MA2SnCl6-based piezoelectric nanogenerator (PENG) with a lithium metal battery (LMB) which also uses the MA2SnCl6-based thin film as the cathode is demonstrated. The MA2SnCl6-based PENG exhibited a high output power density of 7.33 μW cm-2 and an excellent mechanical durability. Further, the MA2SnCl6 as a cathode in LMB recorded the highest specific capacity of 589.98 mAh g-1. Moreover, 1 nm-thick Al2O3 coating on the MA2SnCl6 surface improved the capacity retention from 16.9% to 75.1% for 100 cycles, indicating its stable performance. Further, the MA2SnCl6-based LMB is charged by the MA2SnCl6-based PENG and utilized as SPU for operating various small-scale electronics (humidity meter, calculator, and LED). This work, not only demonstrates the immediate feasibility of MHPs toward high-capacity batteries and energy harvesters, but also provides an insight into the general design principles of MHP-based devices. © 2022, The Authors. All rights reserved.

关键词： Cathodes

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Inverse designing metamaterials with programmable nonlinear functional responses in graph space

arXiv

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arXiv 2024年

作者： Maurizi, Marco Xu, Derek Wang, Yu-Tong Yao, Desheng Hahn, David Oudich, Mourad Satpati, Anish Bauchy, Mathieu Wang, Wei Sun, Yizhou Jing, Yun Zheng, Xiaoyu Rayne Department of Materials Science and Engineering University of California Berkeley Berkeley94720 United States Department of Computer Science University of California Los Angeles Los Angeles90095 United States Graduate Program in Acoustics Penn State University PA16802 United States Universite’ de Lorraine CNRS Institut Jean Lamour NancyF-54000 France Department of Civil and Environmental Engineering University of California Los Angeles Los Angeles90095 United States

Material responses to static and dynamic stimuli, represented as nonlinear curves, are design targets for engineering functionalities like structural support, impact protection, and acoustic and photonic bandgaps. Three-dimensional metamaterials offer significant tunability due to their internal structure, yet existing methods struggle to capture their complex behavior-to-structure relationships. We present GraphMetaMat, a graph-based framework capable of designing three-dimensional metamaterials with programmable responses and arbitrary manufacturing constraints. Integrating graph networks, physics biases, reinforcement learning, and tree search, GraphMetaMat can target stress-strain curves spanning four orders of magnitude and complex behaviors, as well as viscoelastic transmission responses with varying attenuation gaps. GraphMetaMat can create cushioning materials for protective equipment and vibration-damping panels for electric vehicles, outperforming commercial materials, and enabling the automatic design of materials with on-demand functionalities. Copyright © 2024, The Authors. All rights reserved.

关键词： Metamaterials

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Photoresponse of Thermally Evaporated Copper Oxide-Based Solar Cells

Photoresponse of Thermally Evaporated Copper Oxide-Based Sol...

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Solar Conference (MENA-SC), Middle East and North Africa

作者： Abdul Hai Alami Mohamad Ayoub Adnan Alashkar Shamma Alasad Ayman Mdallal Siren Khuri Haya Aljaghoub Sustainable and Renewable Energy Engineering Department Sustainable Energy & Power Systems Research Centre University of Sharjah Sharjah United Arab Emirates Materials Science and Engineering PhD Program American University of Sharjah Sharjah United Arab Emirates Mechancial Engineering Department American University of Sharjah Sharjah United Arab Emirates Sustainable Energy & Power Systems Research Centre University of Sharjah Sharjah United Arab Emirates Industrial Engineering and Engineering Management Department University of Sharjah Sharjah United Arab Emirates

This study reports on the fabrication and characterization of a copper oxide (CuO)-based photoactive cell. Copper was thermally evaporated onto two substrates and post-treated using chemical and thermal treatments to obtain different semiconducting types of CuO. Absorption measurements were conducted to obtain the bandgaps of CuO, which were found to be 1.51 eV and 1.21 eV, for the chemically and thermally treated CuO, respectively. Finally, a chronoamperometry test was conducted to confirm the photoresponse of the cell, which showed a doubling of output current values under light conditions compared to dark conditions.

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Metallization of colloidal crystals

arXiv

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arXiv 2021年

作者： Ehlen, Ali Lopez-Rios, Hector de la Cruz, Monica Olvera Applied Physics Program Northwestern University Department of Materials Science and Engineering Northwestern University

Colloidal crystals formed by size-asymmetric binary particles co-assemble into a wide variety of colloidal compounds with lattices akin to ionic crystals. Recently, a transition from a compound phase with a sublattice of small particles to a metal-like phase in which the small particles are delocalized has been predicted computationally and observed experimentally. In this colloidal metallic phase, the small particles roam the crystal maintaining the integrity of the lattice of large particles, as electrons do in metals. A similar transition also occurs in superionic crystals, termed sublattice melting. Here, we use energetic principles and a generalized molecular dynamics (MD) model of a binary system of functionalized nanoparticles (NPs) to analyze the transition to sublattice delocalization in different co-assembled crystal phases as a function of temperature (T), number of grafted chains on the small particles, and number ratio between the small and large particles ns:nl. We find that ns:nl is the primary determinant of crystal type due to energetic interactions and interstitial site filling, while the number of grafted chains per small particle determines the stability of these crystals. We observe first-order sublattice delocalization transitions as T increases, in which the host lattice transforms from low- to high-symmetry crystal structures, including A20 → BCT → BCC, Ad → BCT → BCC, and BCC → BCC/FCC → FCC transitions and lattices. Analogous sublattice transitions driven primarily by lattice vibrations have been seen in some atomic materials exhibiting an insulator-metal transition also referred to as metallization. We also find minima in the lattice vibrations and diffusion coefficient of small particles as a function of ns:nl, indicating enhanced stability of certain crystal structures for ns:nl values that form compounds. © 2021, CC BY.

关键词： Molecular dynamics

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Improving iPSC Differentiation Using a Nanodot Platform

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ACS Applied materials and Interfaces 2024年第28期16卷 36030-36046页

作者： Chiew, Men Yee Wang, Erick Lan, Kuan-Chun Lin, Yan-Ren Hsueh, Yu-Huan Tu, Yuan-Kun Liu, Chu-Feng Chen, Po-Chun Lu, Huai-En Chen, Wen Liang Center for Regenerative Medicine and Cellular Therapy National Yang Ming Chiao Tung University Hsinchu300 Taiwan Department of Biological Science and Technology National Yang Ming Chiao Tung University Hsinchu300 Taiwan College of Biological Science and Technology Industrial Ph. D. Program National Yang Ming Chiao Tung University Hsinchu300 Taiwan Kyoto University Kyoto606-8397 Japan Department of Emergency and Critical Care Medicine Changhua Christian Hospital Changhua500 Taiwan Department of Post Baccalaureate Medicine College of Medicine National Chung Hsing University Taichung402 Taiwan School of Medicine Kaohsiung Medical University Kaohsiung807 Taiwan School of Medicine Chung Shan Medical University Taichung402 Taiwan College of Biological Science and Technology National Yang Ming Chiao Tung University Hsinchu300 Taiwan Department of Orthopedic Surgery E-Da Hospital I-Shou University Kaohsiung824 Taiwan Emergency Medicine Department Kaohsiung Chang Gung Memorial Hospital Kaohsiung833 Taiwan Ph. D. Degree Program of Biomedical Science and Engineering National Yang Ming Chiao Tung University Hsinchu300 Taiwan Institute of Materials Science and Engineering National Taipei University of Technology Taipei106 Taiwan Institute of Biochemistry and Molecular Biology National Yang Ming Chiao Tung University Hsinchu300 Taiwan Bioresource Collection and Research Center Food Industry Research and Development Institute Hsinchu City300 Taiwan

Differentiation of induced pluripotent stem cells (iPSCs) is an extremely complex process that has proven difficult to study. In this research, we utilized nanotopography to elucidate details regarding iPSC differentiation by developing a nanodot platform consisting of nanodot arrays of increasing diameter. Subjecting iPSCs cultured on the nanodot platform to a cardiomyocyte (CM) differentiation protocol revealed several significant gene expression profiles that were associated with poor differentiation. The observed expression trends were used to select existing small-molecule drugs capable of modulating differentiation efficiency. BRD K98 was repurposed to inhibit CM differentiation, while iPSCs treated with NSC-663284, carmofur, and KPT-330 all exhibited significant increases in not only CM marker expression but also spontaneous beating, suggesting improved CM differentiation. In addition, quantitative polymerase chain reaction was performed to determine the gene regulation responsible for modulating differentiation efficiency. Multiple genes involved in extracellular matrix remodeling were correlated with a CM differentiation efficiency, while genes involved in the cell cycle exhibited contrasting expression trends that warrant further studies. The results suggest that expression profiles determined via short time-series expression miner analysis of nanodot-cultured iPSC differentiation can not only reveal drugs capable of enhancing differentiation efficiency but also highlight crucial sets of genes related to processes such as extracellular matrix remodeling and the cell cycle that can be targeted for further investigation. Our findings confirm that the nanodot platform can be used to reveal complex mechanisms behind iPSC differentiation and could be an indispensable tool for optimizing iPSC technology for clinical applications. © 2024 The Authors. Published by American Chemical Society.

关键词： Efficiency

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