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RSC Applied Interfaces 2024年第5期1卷 1077-1092页

作者： Quilty, Calvin D. Marin Bernardez, Edelmy J. Nicoll, Andrew Hossain, MD Jamil Kingan, Arun Arnot, David J. Mohamed, Hafsa A. Tong, Xiao Jaye, Cherno Fischer, Daniel A. Wang, Lei Qi, Yue Takeuchi, Esther S. Marschilok, Amy C. Yan, Shan Bock, David C. Takeuchi, Kenneth J. Department of Chemistry Stony Brook University Stony Brook 11794 NY United States Institute of Energy: Sustainability Environment and Equity (I:SEE) Stony Brook University Stony Brook 11794 NY United States School of Engineering Brown University Providence 02912 RI United States Department of Materials Science and Chemical Engineering Stony Brook University Stony Brook 11794 NY United States Science Undergraduate Laboratory Internship (SULI) Program Brookhaven National Laboratory Upton 11973 NY United States Department of Chemistry University of Rochester Rochester 14627 NY United States Department of Chemistry The College of Wooster Wooster 44691 OH United States Center for Functional Nanomaterials Brookhaven National Laboratory Upton 11973 NY United States Material Measurement Laboratory National Institute of Standards and Technology Gaithersburg 20899 MD United States Interdisciplinary Science Department Brookhaven National Laboratory Upton 11973 NY United States

Facilitating widespread adoption of electric vehicles will require next-generation battery systems that can operate reliably over a large temperature range, at high operating voltage, and under fast charging rates. Herein, a novel class of nonflammable fluorinated ester-based local high concentration electrolytes (LHCEs) are described. When cycled in commercially relevant graphite/LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) pouch cells, these electrolytes demonstrate improved capacity retention compared to carbonate-based electrolytes under multiple usage conditions including high voltage (4.5 V), fast charge (4C, 15 minutes), and low temperature (−20 °C) without sacrificing capacity retention at elevated temperature (40 °C). Low carbon, high fluoride cathode electrolyte interphases formed by the LHCE system yield a significant reduction in charge transfer impedance during cycling and contribute to capacity retention. These results demonstrate that using fluorinated esters in a LHCE modality enables creation of a new class of nonflammable electrolytes that can successfully operate over broad operating conditions. © 2024 RSC.

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Nano-Engineered Ga-Doped Llzo Electrolytes: A Leap Toward High-Performance Solid-State Batteries

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SSRN 2023年

作者： Jo, Seong-Jun Jeon, Young-Gue Hwang, Sang-Yeop Lim, Sung-Hwan Kumar, Ramachandran Vasant Kim, Kwang-Bum Kim, Hyun-Kyung Department of Battery Convergence Engineering Kangwon National University 1 Kangwondaehak-gil Chuncheon24341 Korea Republic of Interdisciplinary Program in Advanced Functional Materials and Devices Development Kangwon National University Chuncheon24341 Korea Republic of Department of Materials Science and Metallurgy University of Cambridge 27 Charles Babbage Road CambridgeCB3 0FS United Kingdom Department of Materials Science and Engineering Yonsei University 134 Shinchon-dong Seodaemoon-gu Seoul120-749 Korea Republic of

Garnet-type Li7La3Zr2O12 (LLZO) Li-ion solid electrolytes are promising candidates for the next generation of safe solid-state batteries. However, the lack of a methodology to control the ceramic powder particle size for obtaining and densifying fast-ion-conducting cubic garnet hinders the application of the Li7La3Zr2O12 as a Li+ ion solid electrolyte. In this study, the doping concentration of Ga, calcination temperature of the Ga-doped LLZO (Ga-LLZO) precursor for achieving nanostructured powders, and the evolution of grain size during sintering conditions are explored to determine the optimum parameters to prepare highly conductive ceramics using the microwave-assisted solvothermal method. The nanostructured precursor (−3 S cm−1) that be employed as a solid electrolyte in a lithium-ion battery. The above approach opens up a new synthesis avenue for making doped Li7La3Zr2O12-type materials with improved properties for energy storage applications. © 2023, The Authors. All rights reserved.

关键词： Solid electrolytes

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Spectroscopic and Interferometric Sum-Frequency Imaging of Strongly Coupled Phonon Polaritons in SiC Metasurfaces

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arXiv 2023年

作者： Niemann, Richarda Mueller, Niclas S. Wasserroth, Sören Lu, Guanyu Wolf, Martin Caldwell, Joshua D. Paarmann, Alexander Fritz-Haber-Institut der Max-Planck-Gesellschaft Faradayweg 4-6 Berlin14195 Germany Department of Mechanical Engineering Vanderbilt University NashvilleTN37235 United States Interdisciplinary Materials Science Graduate Program Vanderbilt University NashvilleTN37235 United States

Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near-field optical microscopy and far-field reflection spectroscopy. Here, we introduce infrared-visible sum-frequency spectro-microscopy as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub-wavelength spatial resolution and highly-resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide-field microscopic detection of the upconverted light. We employ this technique to image hybridization and strong coupling of localized and propagating surface phonon polaritons in metasurfaces of SiC micropillars. Spectro-microscopy allows us to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, we directly visualize how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. We further observe the formation of edge states at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. Our approach is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non-perturbative tool to image polariton hybridization and propagation. © 2023, CC BY.

关键词： Polariton

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Enhancing Zinc Electrode Stability Through Pre-Desolvation and Accelerated Charge Transfer Via a Polyimide Interface

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SSRN 2023年

作者： Lai, Chi-Yu Liao, Yin-Song Ku, Hao-Yu Jao, Wen-Yang Gull, Sanna Chen, Han-Yi Chou, Jyh-Pin Hu, Chi-Chang Department of Chemical Engineering National Tsing Hua University Hsinchu300044 Taiwan Tsing Hua Interdisciplinary Program National Tsing Hua University Hsinchu300044 Taiwan Department of Materials Science and Engineering National Tsing Hua University Hsinchu300044 Taiwan Department of Physics National Changhua University of Education Changhua50074 Taiwan

Aqueous zinc-based energy storage devices possess superior safety, cost-effectiveness, and high energy density;however, dendritic growth and side reactions on the zinc electrode curtail their widespread applications. In this study, we mitigate these issues by introducing a polyimide (PI) nanofabric interfacial layer onto the zinc substrate. Simulations reveal that the PI nanofabric promotes a pre-desolvation process, effectively desolvating hydrated zinc ions from Zn(H2O)62+ to Zn(H2O)42+ before approaching zinc surface. The exposed zinc ion in Zn(H2O)42+ provides an accelerated charge transfer process and reduces the activation energy for zinc deposition from 40 to 21 kJ mol−1. The PI nanofabric also acts as a protective barrier, reducing water molecule interactions and side reactions at the electrode. The PI-Zn symmetric cell exhibits remarkable cycling stability over 1200 h, maintaining a dendrite-free morphology and minimal byproduct formation. Moreover, the cell exhibits high stability and low voltage hysteresis even under high current densities (20 mA cm−2, 10 mAh cm−2) thanks to the three-dimensional porous structure of PI nanofabric. When integrated into full cells, the PI-Zn||AC hybrid zinc-ion capacitor and PI-Zn||MnVOH@SWCNT zinc-ion battery achieve impressive lifespans of 15000 and 600 cycles with outstanding capacitance retention. This approach paves a novel avenue for high-performance zinc metal electrodes. © 2023, The Authors. All rights reserved.

关键词： Charge transfer

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A First-Principles and Calphad-Assisted Phase-Field Model for Microstructure Evolution: Application to Mo-V Binary Alloy Systems

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SSRN 2023年

作者： Thakur, Abhishek Kumar Kovacevic, Sasa Manga, Venkateswara Rao Deymier, Pierre Alix Muralidharan, Krishna Department of Materials Science and Engineering University of Arizona TucsonAZ85721 United States Department of Civil and Environmental Engineering Imperial College London LondonSW7 2AZ United Kingdom Lunar and Planetary Laboratory University of Arizona TucsonAZ85721 United States Graduate Interdisciplinary Program in Applied Mathematics India

A multiscale computational framework combining the first-principles calculations and the CALPHAD approach with the phase-field method is presented to simulate the microstructure evolution in multicomponent steel alloys. We demonstrate the potential of the framework by predicting the microstructural evolution in elastically periodic arrays of the Mo-V binary sub-system. The framework utilizes the first-principles calculations using special quasi-random structures. Hitherto unavailable thermodynamic and material properties of the alloy are obtained by employing the first-principles calculations and the CALPHAD approach and fed into the phase-field model to predict the microstructure evolution at different temperatures within the miscibility gap region. In addition to the temperature and cooling rates, the model incorporates the role of mechanical fields in decomposition kinetics in the Mo-V binary alloy system. Regimes for temperatures and cooling rates at which spinodal decomposition occurs are identified. Applying external loading leads to directional phase separation in the Mo-V binary system. The elastic inhomogeneity in terms of material properties between the two phases initiates the directional alignment while eigenstrains and applied external loading control the degree of alignment. The framework developed is general and extendable to higher multicomponent sub-systems in steel alloys. © 2023, The Authors. All rights reserved.

关键词： Temperature

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6-Methoxyquinoline Immobilized Nylon Sensor for Monitoring Chloride Concentration in Reinforced Concrete

SSRN

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SSRN 2023年

作者： Jeong, Hoseong Jung, Byung Jun Kim, Jae Hyun Kim, Kang Su Department of Architectural Engineering and Smart City Interdisciplinary Major Program University of Seoul 163 Seoulsiripdaero Dongdaemun-gu Seoul02504 Korea Republic of Department of Materials Science and Engineering University of Seoul 163 Seoulsiripdaero Dongdaemun-gu Seoul02504 Korea Republic of Department of Architectural Engineering University of Seoul 163 Siripdae-ro Dongdaemun-gu Seoul02504 Korea Republic of

An excess in the threshold concentration of chloride in concrete leads to the initiation of reinforcement corrosion, which in turn results in a reduction in the load-bearing capacity of reinforced concrete(RC) structures. Accordingly, the chloride concentration of RC is periodically investigated via a destructive method, but this process is time-consuming, labor-intensive, and costly. In order to overcome the limitations, this study sought to develop an optical chloride sensor that can be used in structural health monitoring. To this end, nylon was functionalized using formaldehyde and epichlorohydrine, after which 6-methoxy quinoline was covalently immobilized to manufacture a sensor. The developed sensor was found to be capable of measuring chloride concentrations (0~5,000mM) and exhibited rapid responsiveness and reversibility. In addition, the developed sensor also showed a stable response even when exposed to the pH 13.4 environment for three months, and it could detect changes in chloride concentration even inside the mortar. © 2023, The Authors. All rights reserved.

关键词： Reinforced concrete

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Leveraging Impurities in Recycled Lead Anodes for Sodium-Ion Batteries

SSRN

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SSRN 2022年

作者： Eaves-Rathert, Janna Moyer-Vanderburgh, Kathleen Wolfe, Kody Zohair, Murtaza Pint, Cary L. Department of Mechanical Engineering Vanderbilt University NashvilleTN37235 United States Interdisciplinary Materials Science Program Vanderbilt University NashvilleTN37235 United States Department of Mechanical Engineering Iowa State University AmesIA50011 United States

In recent years, the supply chain shock due to the rapid rise of the lithium-ion battery has made alternative chemistries, such as sodium-ion batteries, appealing for low-cost and large-scale energy storage. Meanwhile, the falling popularity of lead acid batteries has potential consequences for the price of scrap lead and its penetration into waste streams. In this work, we upcycle lead alloys from a used lead acid battery into a next-generation sodium-ion system for ultra-low-cost rechargeable batteries. Through evaluation of sodium storage capacity and rate capability, we study the rich interplay of Pb-Sb-Sn microstructure and properties which can be controlled through simple heat treatment of unrefined powders to reach a maximum specific capacity of 522 mAh.g-1. When cycled in the presence of glyme-based electrolytes, the ternary alloys nanostructure to facilitate an optimal balance of power and cycle life. These findings that demonstrate how defects can be leveraged to improve performance bring exciting implications for reducing cost and mitigating volume expansion in other high-value commodities, like tin or silicon. © 2022, The Authors. All rights reserved.

关键词： Lead acid batteries

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Defect engineering Centrosymmetric 2D Material Flexocatalysts

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Small 2024年第31期20卷 2401116-2401116页

作者： Chen, Yu-Ching Chen, Po-Han Liao, Yin-Song Chou, Jyh-Pin Wu, Jyh Ming Department of Materials Science and Engineering National Tsing Hua University 101 Section 2 Kuang Fu Road Hsinchu300 Taiwan Ph.D. Program in Prospective Functional Materials Industry National Tsing Hua University 101 Section 2 Kuang Fu Road Hsinchu300 Taiwan Tsing Hua Interdisciplinary Program National Tsing Hua University 101 Section 2 Kuang Fu Road Hsinchu300 Taiwan Department of Physics National Changhua University of Education No. 1 Jin-De Road Changhua500 Taiwan High Entropy Materials Center National Tsing Hua University 101 Section 2 Kuang Fu Road Hsinchu300 Taiwan

In this study, the flexoelectric characteristics of 2D TiO2 nanosheets are examined. The theoretical calculations and experimental results reveal an excellent strain-induced flexoelectric potential (flexopotential) by an effective defect engineering strategy, which suppresses the recombination of electron–hole pairs, thus substantially improving the catalytic activity of the TiO2 nanosheets in the degradation of Rhodamine B dye and the hydrogen evolution reaction in a dark environment. The results indicate that strain-induced bandgap reduction enhances the catalytic activity of the TiO2 nanosheets. In addition, the TiO2 nanosheets degraded Rhodamine B, with kobs being ≈1.5 × 10−2 min−1 in dark, while TiO2 nanoparticles show only an adsorption effect. 2D TiO2 nanosheets achieve a hydrogen production rate of 137.9 µmol g−1 h−1 under a dark environment, 197% higher than those of TiO2 nanoparticles (70.1 µmol g−1 h−1). The flexopotential of the TiO2 nanosheets is enhanced by increasing the bending moment, with excellent flexopotential along the y-axis. Density functional theory is used to identify the stress-induced bandgap reduction and oxygen vacancy formation, which results in the self-dissociation of H2O on the surface of the TiO in the dark. The present findings provide novel insights into the role of TiO2 flexocatalysis in electrochemical reactions. © 2024 Wiley-VCH GmbH.

关键词： Titanium dioxide

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Titanium dioxide/nitrogen-doped graphene-biopolymer based nanocomposite films for pollutant photodegradation and laser desorption ionization mass spectrometry of biomarkers

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Nano-Structures and Nano-Objects 2024年 38卷

作者： Siripongpreda, Tatiya Jiraborvornpongsa, Noppakhate Composto, Russell J. Rodthongkum, Naddudda Nanoscience and Technology Interdisciplinary Program Chulalongkorn University Phayathai Road Wangmai Patumwan Bangkok 10330 Thailand Metallurgy and Materials Science Research Institute Chulalongkorn University Phayathai Road Wangmai Patumwan Bangkok 10330 Thailand Photocatalysts for Clean Environment and Energy Research Unit Faculty of Science Chulalongkorn University Phayathai Road Wangmai Patumwan Bangkok 10330 Thailand Department of Materials Science and Engineering University of Pennsylvania Philadelphia 19104 PA United States Center of Excellence in Responsive Wearable Materials Chulalongkorn University Soi Chula 12 Phayathai Road Pathumwan Bangkok 10330 Thailand

Titanium dioxide (TiO2)/nitrogen-doped graphene (NG) nanocomposite is prepared via a solvent-free hydrothermal reaction. The resulting TiO2/NG materials exhibit a reduction of the band gap energy compared to pristine ... 详细信息

Titanium dioxide (TiO₂)/nitrogen-doped graphene (NG) nanocomposite is prepared via a solvent-free hydrothermal reaction. The resulting TiO₂/NG materials exhibit a reduction of the band gap energy compared to pristine TiO₂ from 3.27 eV to 2.69 eV. These materials are characterized by scanning transmission electron microscopy (STEM), energy dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). To prepare biopolymer films with photocatalytic properties, TiO₂ and NG are mixed with biodegradable chitosan and spin-coated on a silicon wafer. Film roughness and thickness are evaluated by atomic force microscopy (AFM). These films are then tested for ciprofloxacin photodegradation by irradiating with visible light. In comparison to the TiO₂/chitosan films, the addition of NG substantially enhances photodegradation efficiency by up to 34 % upon the addition of 5 % w/w of NG. Furthermore, this film is shown to be a good substrate for biomarker detection using laser desorption ionization mass spectrometry (LDI-MS). In summary, this nanocomposite-biopolymer film provides good photocatalytic activity towards ciprofloxacin degradation and enhances the ionization efficiency of peptide biomarkers in LDI-MS owing to high efficiency of laser absorption/desorption. This nanocomposite film might be useful for environmental-related and medical application. © 2024 Elsevier B.V.

关键词： LDI-MS Nanocomposite film Nitrogen-doped graphene Photodegradation Titanium dioxide

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Naked-eye observation of water-forming reaction on palladium etalon:transduction of gas-matter reaction into light-matter interaction

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PhotoniX 2023年第1期4卷 349-363页

作者： Jongsu Lee Eui-Sang Yu Taehyun Kim In Soo Kim Seok Chung Seung Jae Kwak Won Bo Lee Yusin Pak Yong-Sang Ryu Sensor System Research Center Korea Institute of Science and TechnologySeoul 02792Republic of Korea Department of Electrical and Computer Engineering Seoul National UniversitySeoul 08826Republic of Korea Smart Materials Research Section Electronics and Telecommunications Research InstituteDaejeon 34129Republic of Korea Department of Micro/Nano Systems Korea University02841 SeoulRepublic of Korea Nanophotonics Research Center Korea Institute of Science and TechnologySeoul 02792Republic of Korea School of Mechanical Engineering Korea UniversitySeoul 02841Republic of Korea School of Chemical and Biological Engineering Seoul National UniversitySeoul 08826Republic of Korea Interdisciplinary Program in Precision Public Health Korea UniversitySeoul 02481Republic of Korea School of Biomedical Engineering Korea UniversitySeoul 02481Republic of Korea

Palladium is the most prominent material in both scientific and industrial research on gas storage,purification,detection,and catalysis due to its unique properties as a catalyst and hydrogen *** the dynamic optical phenomena of palladium reacting with hydrogen,transduction of the gas-matter reaction into light-matter interaction is attempted to visualize the dynamic surface chemistry and reaction *** simple geometry of the metal-dielectric-metal structure,Fabry-Perot etalon,is employed for a colorimetric reactor,to display the catalytic reaction of the exposed gas via water-film/bubble formation at the dielectric/palladium *** adsorption/desorption behavior and catalytic reaction of hydrogen and oxygen on the palladium surface display highly repeatable and dramatic color changes based on two distinct water formation trends:the foggy effect by water bubbles and the whiteout effect by water film *** and experiments demonstrate the robustness of the proposed Fabry-Perot etalon as an excellent platform for monitoring the opto-physical phenomena driven by heterogeneous catalysis.

关键词： Palladium Hydrogen Oxygen Fabry-Perot resonators Colorimetric sensors Water-forming reaction

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