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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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Driving selective photoelectrocatalytic oxidation of seawater to oxygen via regulating interfacial water structures on titanium oxides

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Chinese Journal of Catalysis 2025年第5期72卷 154-163页

作者： Qisen Jia Yanan Wang Yan Zhao Zhenming Tian Luyao Ren Xuejing Cui Guangbo Liu Xin Chen Wenzhen Li Luhua Jiang Nanomaterials&Electrocatalysis Laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation Southwest Petroleum UniversityChengdu 610500SichuanChina Center for Computational Chemistry and Molecular Simulation College of Chemistry and Chemical EngineeringSouthwest Petroleum UniversityChengdu 610500SichuanChina Department of Chemical&Biological Engineering Iowa State UniversityAmesIA 50011–1098United States

Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic ***,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC ***,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the *** work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.

关键词： Photoelectrocatalysis Seawater splitting Selectivity Interfacial water structure Energy band structure

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Quantitative Analysis of Sodium Metal Deposition and Interphase in Na Metal Batteries

arXiv

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arXiv 2023年

作者： Sayahpour, Baharak Li, Weikang Bai, Shuang Lu, Bingyu Han, Bing Chen, Yu-Ting Deysher, Grayson Parab, Saurabh Ridley, Phillip Raghavendran, Ganesh Nguyen, Long Hoang Bao Zhang, Minghao Meng, Ying Shirley Materials Science and Engineering Program University of California San DiegoCA92093 United States Department of NanoEngineering University of California San DiegoCA92093 United States Pritzker School of Molecular Engineering University of Chicago ChicagoIL60637 United States

Sodium-ion batteries exhibit significant promise as a viable alternative to current lithium-ion technologies owing to their sustainability, low cost per energy density, reliability, and safety. Despite recent advancements in cathode materials for this category of energy storage systems, the primary challenge in realizing practical applications of sodium-ion systems is the absence of an anode system with high energy density and durability. Although Na metal is the ultimate anode that can facilitate high-energy sodium-ion batteries, its use remains limited due to safety concerns and the high-capacity loss associated with the high reactivity of Na metal. In this study, titration gas chromatography is employed to accurately quantify the sodium inventory loss in ether- and carbonate-based electrolytes. Uniaxial pressure is developed as a powerful tool to control the deposition of sodium metal with dense morphology, thereby enabling high initial coulombic efficiencies. In ether-based electrolytes, the Na metal surface exhibits the presence of a uniform solid electrolyte interphase layer, primarily characterized by favorable inorganic chemical components with close-packed structures. The full cell, utilizing a controlled electroplated sodium metal in ether-based electrolyte, provides capacity retention of 91.84% after 500 cycles at 2C current rate and delivers 86 mAh/g discharge capacity at 45C current rate, suggesting the potential to enable Na metal in the next generation of sodium-ion technologies with specifications close to practical requirements. © 2023, CC BY-NC-ND.

关键词： Ethers

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Efficient Predictions of Formation Energies and Convex Hulls from Density Functional Tight Binding Calculations

SSRN

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SSRN 2022年

作者： Kumar, Anshuman Ali, Zulfikhar A. Wong, Bryan M. Materials Science & Engineering Program University of California Riverside RiversideCA92521 United States Department of Physics & Astronomy University of California Riverside RiversideCA92521 United States Materials Science & Engineering Program Department of Chemical & Environmental Engineering Department of Physics & Astronomy Department of Chemistry University of California Riverside RiversideCA92521 United States

Defects in materials significantly alter their electronic and structural properties, which affect the performance of electronic devices, structural alloys, and functional materials. However, calculating all the possible defects in complex materials with conventional Density Functional Theory (DFT) can be computationally prohibitive. To enhance the efficiency of these calculations, we interfaced Density Functional Tight Binding (DFTB) with the Clusters Approach to Statistical Mechanics (CASM) software package for the first time to calculate formation energies and convex hulls. Using SiC and ZnO as representative examples, we show that DFTB gives accurate results and can be a computationally cheaper alternative to DFT. Our DFTB+CASM implementation allows for an efficient exploration (up to an order of magnitude faster than DFT) of formation energies and convex hulls, which researchers can use to probe other complex systems. © 2022, The Authors. All rights reserved.

关键词： Density functional theory

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Field-controlled dynamics of skyrmions and monopoles

arXiv

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arXiv 2023年

作者： Tai, Jung-Shen B. Hess, Andrew J. Wu, Jin-Sheng Smalyukh, Ivan I. Department of Physics Chemical Physics Program University of Colorado BoulderCO80309 United States Department of Electrical Computer and Energy Engineering Materials Science and Engineering Program Soft Materials Research Center University of Colorado BoulderCO80309 United States Renewable and Sustainable Energy Institute National Renewable Energy Laboratory University of Colorado BoulderCO80309 United States

Magnetic monopoles, despite their ongoing experimental search as elementary particles, have inspired the discovery of analogous excitations in condensed matter systems. In chiral condensed matter systems, emergent monopoles are responsible for the onset of transitions between topologically distinct states and phases, like in the case of transitions from helical and conical phase to A-phase comprising periodic arrays of skyrmions. By combining numerical modeling and optical characterizations, we describe how different geometrical configurations of skyrmions terminating at monopoles can be realized in liquid crystals and liquid crystal ferromagnets. We demonstrate how such complex structures can be effectively manipulated by external magnetic and electric fields. Furthermore, we discuss how our findings may hint at similar dynamics in other physical systems, and their potential applications. © 2023, CC BY.

关键词： Liquid crystals

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Dual Functionality of Carbazole-Based Phosphonic Acid Molecules Enables Efficient Hole Transport Layer-Free Perovskite Light-Emitting Diodes

SSRN

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SSRN 2024年

作者： Lai, Yin-Ti Chen, Chiung-Han Yu, Ming-Hsuan Kuo, Hsing-Yu Ni, I-Chih Lin, Bi-Hsuan Kim, Hobeom Kuo, Chi-Ching Lu, Yu-Jung Chueh, Chu-Chen Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Research Center for Applied Sciences Academia Sinica Taipei11529 Taiwan Department of Physics National Taiwan University Taipei10617 Taiwan Graduate Institute of Photonics and Optoelectronics National Taiwan University Taipei10617 Taiwan National Synchrotron Radiation Research Center Hsinchu30076 Taiwan School of Materials Science and Engineering Gwangju Institute of Science and Technology Korea Republic of Department of Molecular Science and Engineering Institute of Organic and Polymeric Materials National Taipei University of Technology Taipei106 Taiwan

Traditionally, perovskite light-emitting diodes (PeLEDs) have used complex and costly hole-transporting layers (HTLs), but these materials pose a significant challenge to commercialization due to their synthetic complexity and energy-intensive deposition processes. Eliminating the use of HTLs can effectively reduce manufacturing costs and simplify device production. Here, we present a simple method to achieve efficient HTL-free devices by exploiting the self-assembly property of carbazole-based phosphonic acid (PACz) molecules to address the issues of poor hole injection and charge imbalance in HTL-free PeLEDs. The results show that the self-assembly property and defect passivation effect of PACz molecules significantly improve the device performance. The self-assembly of some molecules on the ITO substrate creates hole-selective contacts and lowers the hole injection barrier. This facilitates hole injection and radiative recombination. Meanwhile, due to the interaction between P=O (and/or halide headgroup) and perovskite, some molecules incorporated in perovskite effectively passivate the uncoordinated Pb2+ and halide vacancies. As a result, efficient HTL-free PeLEDs were realized by incorporating PACz molecules into perovskites. © 2024, The Authors. All rights reserved.

关键词： Perovskite

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Three-dimensional morphology of an ultrafine Al-Si eutectic produced via laser rapid solidification

arXiv

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arXiv 2023年

作者： Zhou, Xinyi Chao, Paul Sloan, Luke Lien, Huai-Hsun Hunter, Allen H. Misra, Amit Shahani, Ashwin J. Engineering Physics Program University of Michigan Ann ArborMI48109 United States Department of Materials Science and Engineering University of Michigan Ann ArborMI48109 United States Michigan Center for Materials Characterization University of Michigan Ann ArborMI48109 United States Department of Chemical Engineering University of Michigan Ann ArborMI48109 United States

Al-Si alloys processed by laser rapid solidification yield eutectic microstructures with ultrafine and interconnected fibers. Such fibrous structures have long been thought to bear resemblance to those formed in impurity-doped alloys upon conventional casting. Here, we show that any similarity is purely superficial. By harnessing high-throughput characterization and computer vision techniques, we perform a three-dimensional analysis of the branching behavior of the ultrafine eutectic and compare it against an impurity-modified eutectic as well as a random fractal (as a benchmark). Differences in the branching statistics point to different microstructural origins of the impurity- and quench-modified eutectic. Our quantitative approach is not limited to the data presented here but can be used to extract abstract information from other volumetric datasets, without customization. © 2023, CC BY.

关键词： Eutectics

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Schwann cells acquire a repair phenotype after assembling into spheroids and show enhanced in vivo therapeutic potential for promoting peripheral nerve repair

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Bioengineering and Translational Medicine 2024年第2期9卷 e10635页

作者： Chen, Shih-Heng Wang, Hsin-Wen Yang, Pei-Ching Chen, Shih-Shien Ho, Chia-Hsin Yang, Pei-Ching Kao, Ying-Chi Liu, Shao-Wen Chiu, Han Lin, Yu-Jie Chuang, Er-Yuan Huang, Jen-Huang Kao, Huang-Kai Huang, Chieh-Cheng Department of Plastic and Reconstructive Surgery Linkou Chang Gung Memorial Hospital Taoyuan Taiwan School of Medicine College of Medicine Chang Gung University Taoyuan Taiwan Institute of Biomedical Engineering National Tsing Hua University Hsinchu Taiwan Graduate Institute of Biomedical Materials and Tissue Engineering College of Biomedical Engineering International Ph.D. Program in Biomedical Engineering Taipei Medical University Taipei Taiwan Cell Physiology and Molecular Image Research Center Taipei Medical University–Wan Fang Hospital Taipei Taiwan Department of Chemical Engineering National Tsing Hua University Hsinchu Taiwan

The prognosis for postinjury peripheral nerve regeneration remains suboptimal. Although transplantation of exogenous Schwann cells (SCs) has been considered a promising treatment to promote nerve repair, this strategy has been hampered in practice by the limited availability of SC sources and an insufficient postengraftment cell retention rate. In this study, to address these challenges, SCs were aggregated into spheroids before being delivered to an injured rat sciatic nerve. We found that the three-dimensional aggregation of SCs induced their acquisition of a repair phenotype, as indicated by enhanced levels of c-Jun expression/activation and decreased expression of myelin sheath protein. Furthermore, our in vitro results demonstrated the superior potential of the SC spheroid-derived secretome in promoting neurite outgrowth of dorsal root ganglion neurons, enhancing the proliferation and migration of endogenous SCs, and recruiting macrophages. Moreover, transplantation of SC spheroids into rats after sciatic nerve transection effectively increased the postinjury nerve structure restoration and motor functional recovery rates, demonstrating the therapeutic potential of SC spheroids. In summary, transplantation of preassembled SC spheroids may hold great potential for enhancing the cell delivery efficiency and the resultant therapeutic outcome, thereby improving SC-based transplantation approaches for promoting peripheral nerve regeneration. © 2023 The Authors. Bioengineering & Translational Medicine published by Wiley Periodicals LLC on behalf of American Institute of chemical Engineers.

关键词： Regenerative Medicine

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Crystallization of POSS in a PEG-Based Multiblock Polyurethane: Toward A Hybrid Hydrogel

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MRS Online Proceedings Library 2021年第1期847卷 59-64页

作者： Jian Wu Qing Ge Kelly A. Burke Patrick T. Mather Chemical Engineering Department and Polymer Program Institute of Materials Science University of Connecticut Storrs USA Department of Macromolecular Science and Engineering Case Western Reserve University Cleveland USA

Building upon earlier success in forming materials with crystalline ordering of POSS via the telechelic architecture with POSS end-capping polyethylene glycols, here we report similar ordering in PEG-POSS thermoplastic polyurethane applicable to a novel hybrid hydrogel. Thus, a unique series of hybrid thermoplastic polyurethanes (TPUs) were synthesized using poly(ethylene glycol) (PEG) as soft segment and incorporating an isobutyl-functionalized POSS diol (TMP POSS diol) in the hard segment. The molecular weight of PEG was systematically varied to include 10, 20, and 35 kDa while the mole ratio of PEG to POSS diol (as chain extender) was chosen as 8:1. The diisocyanate employed for TPU polymerization was 4, 4'-methylenebis(phenyl-isocyanate) (MDI). Wide-angle X-ray diffraction (WAXD) studies revealed that both the hydrophilic soft segments (PEG) and hydrophobic hard segments (POSS) can form crystalline structures driven by micro-phase separation, itself due to thermodynamic incompatibility. Differential scanning calorimetry (DSC) and rheological studies revealed that thermal history is important in controlling the crystallization of a POSS-rich nanophase. Increasing the cooling rate monotonically decreases the crystallinity of POSS-rich phase and results in a decrease in the ultimate dynamic storage modulus following POSS crystallization and an increase of the loss angle for temperatures above Tm of PEG and below Tm of POSS. We conclude that both composition and thermal history are key factors in determing the internal network built by the POSS nanophase, which will have a significant influence on the properties of the resulting hybrid hydrogels now being studied.

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A Hybrid System Combining Direct Contact Membrane Distillation (Dcmd) and Electrochemical Switched Ion Exchange (Esix) for Efficient Lithium Recovery from Simulated Brine

SSRN

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SSRN 2023年

作者： Gulied, Mona Zavahir, Sifani Elmakki, Tasneem Park, Hyunwoong Shon, Hokyong Han, Dong Suk Center for Advanced Materials Qatar University Doha Qatar Materials Science and Technology Program College of Arts and Science Qatar University Doha Qatar School of Energy Engineering Kyungpook National University Daegu41566 Korea Republic of ARC Research Hub for Nutrients in a Circular Economy Center for Technology in Water and Wastewater School of Civil and Environmental Engineering Faculty of Engineering and IT University of Technology SydneyNSW2007 Australia Department of Chemical Engineering College of Engineering Qatar University Doha Qatar

Recovering valuable elements such as lithium (Li) from seawater reverse osmosis (SWRO) brine is crucial for building a sustainable economy due to its high storage density, making it an ideal material for energy storage. In this study, a novel hybrid system that combines direct contact membrane distillation (DCMD) and electrochemical switched ion exchange (ESIX) was designed to achieve simultaneous SWRO brine enrichment and Li recovery. The DCMD process concentrated the SWRO brine using electrospun nanofiber membranes (ENMs) made of polyvinylidene fluoride (PVDF), with the incorporation of reduced graphene oxide (rGO) nanoparticles enhancing the morphological, thermal, and mechanical stability of the PVDF ENMs. The water contact angle (WCA) of the 1-rGO/PVDF ENM was 142.08°, indicating an improved hydrophobic property that resulted in the recovery of 12% freshwater from simulated SWRO brine and a 2.4-fold increase in Li+ concentration. The 1-rGO/PVDF ENM exhibited stable performance, with an 11% reduction in WCA after 15 hours of brine concentration. In the hybrid operation, a Li-selective LiAlO2 electrode, coupled with an activated carbon counter electrode, demonstrated remarkable Li recovery for Li capture solutions enriched by the rGO-PVDF membrane in the DCMD step. Compared to the Li concentration in the DCMD feed, sequential Li capture and release cycles recovered 91.8% of Li, highlighting the critical role of the hybrid mode operation in concentrating Li from simulated brine solutions. © 2023, The Authors. All rights reserved.

关键词： Hybrid systems

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