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Macromolecule-Enriched Solvation Enabling High-Voltage Sodium-Ion Batteries

Angewandte Chemie 2025年

作者： Zhiming Zhao Chen Liu Tianxing Lai Zehao Cui Arumugam Manthiram Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin Austin TX 78712 USA

Sodium-ion batteries (SIBs) are emerging as a viable alternative for sustainable and cost-effective energy storage, yet their energy density is curtailed by relatively low voltage outputs (< 4 V) due to the lack of high-voltage electrolytes. Here, for the first time, we describe a high-voltage Na + electrolyte featuring a macromolecule-enriched solvation architecture. The vulnerable small molecules in the Na + solvation shell are replaced by macro polyamide (PA) molecules with high thermodynamic resilience, ensuring a wide electrochemical stability window for the electrolytes with suppressed oxidative/reductive decomposition. Concomitantly, the anions engage in H-bonding with the amido groups of PA, which not only stabilizes the anions against hydrolysis, but also delivers a high Na + transference number of 0.93. Importantly, the nitrogen-rich composition of the macromolecule-enriched electrolyte (MEE) fosters the formation of robust nitride interphases that impart enduring stability to both the cathode and anode. As a result, the hard carbon (HC) || NaNi 1/3 Fe 1/3 Mn 1/3 O 2 (NFM) full cells demonstrate significant rechargeability even with an ultrahigh cutoff voltage of 4.4 V. Our approach distinctively avoids the use of fluorinated molecules typically found in (localized-) high-concentration electrolytes, presenting a novel principle that could revolutionize high-voltage electrolyte design.

关键词： Hard carbon anode High-voltage electrolyte Layered oxide cathode Sodium-ion batteries Solvation structure

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Scalable Membraneless Direct Liquid Fuel Cells Based on a Catalyst-Selective Strategy

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Energy & Environmental materials 2018年第1期1卷 13-19页

作者： Xingwen Yu Arumugam Manthiram Materials Science&Engineering Program and Texas Materials Institute The University of Texas at AustinAustinTX 78712USA

This perspective presents a membraneless direct liquid fuel cell(DLFC)concept based on a catalyst-selective *** membraneless DLFCs are operated at low temperatures by employing a non-precious cathode catalyst with a high catalytic *** uniqueness is that the inexpensive cathode catalyst only catalyzes the oxygen reduction reaction but does not catalyze the oxidation reaction of a specific ***,during the operation of DLFCs,the liquid fuel can enter the cathode freely without any concern of fuel *** catalyst-selective approach tactfully avoids the use of high-cost or technically unviable ion-exchange polymer membranes in *** catalyst-selective operating principle also overcomes the scalability issue of the traditional laminar-flow membraneless *** a proper management of the anode and cathode catalysts in the cell,a variety of inexpensive,renewable alcohols,and small-molecule organics can be employed as anode *** innovative approach of membraneless alkaline DLFCs offers a great opportunity for the development of inexpensive energy-generation systems for both mobile and stationary *** addition to summarizing the principle and the research progress of the unique membraneless DLFC platform,the challenges and future research directions are presented.

关键词： catalyst uniqueness overcome

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Forward/reverse dc bias or ac electroluminescence in poly(p-phenylene vinylene) prepared via sulfonium-salt and xanthate routes

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SYNTHETIC METALS 1997年第1-3期85卷 1291-1292页

作者： Kasim, RK Elsenbaumer, RL Materials Science & Engineering Program The University of Texas at Arlington Arlington Texas 76019 USA

In light-emitting diodes (LEDs) of standard configuration - Indium-Tin-Oxide (ITO)/polymer/metal, we observed light emission under ac or forward/reverse de bias, using poly(p-phenylene vinylenes) prepared via the sulfonium salt (S-PPV) or xanthate (X-PPV) routes as active electroluminescent layers. S-PPV devices exhibited approximately symmetrical current-voltage characteristics under forward and reverse de bias with the same onset voltage. The electroluminescence (EL) spectra either under a de forward/reverse bias or ac were identical. X-PPV showed EL under reverse bias at higher voltage than in forward bias. Symmetrical current-voltage characteristics in S-PPV devices is attributed to ionic impurities present in the polymer.

关键词： electroluminescence light emitting diodes poly(phenylene vinylene)

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A mini review on two-dimensional nanomaterial assembly

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Nano Research 2020年第5期13卷 1179-1190页

作者： Zhiwei Fang Qiyu Xing Desiree Fernandez Xiao Zhang Guihua Yu Materials Science and Engineering Program and Department of Mechanical Engineering The University of Texas at AustinAustinTexas 78712USA 2 School of Chemistry and Materials ScienceUniversity of Science&Technology of ChinaHefei 230026China

Two-dimensional(2D)nanomaterials have attracted a great deal of attention since the discovery of graphene in 2004,due to their intriguing physicochemical properties and wide-ranging applications in catalysis,energy-related devices,electronics and *** maximize the potential of 2D nanomaterials for their technological applications,controlled assembly of 2D nanobulding blocks into integrated systems is critically *** mini review summarizes the reported strategies of 2D materials-based assembly into integrated functional nanostructures,from in-situ assembly method to post-synthesis *** applications of 2D assembled integrated structures are also covered,especially in the areas of energy,electronics and sensing,and we conclude with discussion on the remaining challenges and potential directions in this emerging field.

关键词： two-dimensional materials assembly self-assembly post-synthesis assembly integrated nanostructures

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NASICON solid electrolyte coated by indium film for all-solid-state Li-metal batteries

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Tungsten 2022年第4期4卷 316-322页

作者： Yi-Jie Liu Ru-Yi Fang David Mitlin Materials Science and Engineering Program and Texas Materials Institute The University of Texas at AustinAustinTX78712USA

The application of all-solid-state Li-metal batteries with solid oxide electrolytes is hindered by interfacial issues,especially the solid electrolyte/Li-metal *** work introduced a uniform indium film layer on the surface of Na^(+)super ionic conductor(NASICON)solid electrolyte Li_(1.5)Al_(0.5)Ge_(1.5)P_(3)O_(12)(LAGP),which promotes the intimate contact between Li metal and solid electrolyte and hinders the side reactions at the *** impedance spectra show that the battery with coated solid electrolyte presents a smaller interfacial resistance and maintains stability after a long cycling *** contrast,the baseline battery with a pure LAGP pellet shows a contact loss after cycling with the vibration of interfacial *** Li symmetric cells with indium-modified solid electrolyte present stable cycling behavior over 400 h at 0.1 and 0.2 mA·cm^(−2).The all-solid-state Li-metal batteries with a Li anode,indium coating LAGP and two kinds of cathodes,namely carbon nanotubes(CNTs)and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),are prepared and *** CNTs cathode for Li-O2 and Li-air batteries has a higher specific capacity than traditional Li-ion battery *** Li-NCM811 batteries deliver an initial Coulombic efficiency of about 75%,with 82%capacity retention after 20 cycles.

关键词： All-solid-state batteries Solid electrolyte Li1.5Al0.5Ge1.5P3O12 Li-metal anode Interfacial chemistry

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Particle impact compatibility assessment of oxygen preheater 304 stainless steel tubes in gaseous oxygen

引用

materials and Design 2025年 254卷

作者： Shunmugasamy, Vasanth C. Chiffoleau, Gwenael J.A. Forsyth, Elliot Laycock, Nicholas J. Kruijer, Alfred Mansoor, Bilal Mechanical Engineering Program Texas A&M University at Qatar Education City Doha Qatar WHA International Inc. Las CrucesNM United States Qatar Shell Research and Technology Center QSTP Doha Qatar Shell Global Solutions International BV The Hague Netherlands Department of Materials Science and Engineering Texas A&M University College StationTX United States

Oxygen preheaters constructed from stainless steel (SS) 304 tubing with multiple bend radius are known to be operated at temperatures > 250 °C, pressures ∼ 50 bar, and gas velocities of 5–10 m/s across process industries. To improve overall efficiency, there is growing interest in raising these operating conditions to 300 °C and 70 bar, which when compared with Compressed Gas Association's recommended Pressure-Velocity design curve, exceed suggested velocity limits for minimizing particle impacts. This necessitates rigorous materials compatibility assessment to mitigate ignition and burnout risks. This work examines particle impact (PI) behavior of SS304 tubes using a custom-built test rig, to evaluate how tube geometry (larger- vs. smaller-radii bends) and operational mode (transient vs. steady flow) affect likelihood of particle ignition and tube kindling. Under transient flow, tubes with larger-radius bends (larger fractional path) exhibited more pronounced iron-particle ignition than those with smaller-radius bends (higher impingement angle), producing molten slag resulting in localized heat-affected zone (∼100 µm) on tube wall. In contrast, no particle ignition occurred under steady flow or when using inert particles. Overall, insights from this study provide a foundation for effective PI testing of curved tubes and supports more informed design and safer operation of oxygen preheaters, when extending beyond conventional guidelines. © 2025 The Author(s)

关键词： Stainless steel

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Sulfur and nitrogen codoped cyanoethyl cellulose-derived carbon with superior gravimetric and volumetric capacity for potassium ion storage

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Carbon Energy 2022年第5期4卷 986-1001页

作者： Guangzeng Cheng Wenzhe Zhang Wei Wang Huanlei Wang Yixian Wang Jing Shi Jingwei Chen Shuai Liu Minghua Huang David Mitlin School of Materials Science and Engineering Ocean University of ChinaQingdaoShandongChina Materials Science and Engineering Program Texas Materials Institute(TMI)The University of Texas at AustinAustinTexasUSA

We fabricated sulfur and nitrogen codoped cyanoethyl cellulose-derived carbons(SNCCs)with state-of-the-art electrochemical performance for potassium ion battery(PIB)and potassium ion capacitor(PIC)*** 0.2,0.5,1,2,5,and 10 A g−1,the SNCC shows reversible capacities of 369,328,249,208,150,and 121 mA h g−1,*** to a high packing density of 1.01 g cm^(−3),the volumetric capacities are also uniquely favorable,being 373,331,251,210,151,and 122 mA h cm^(−3)at these currents,*** also shows promising initial Coulombic efficiency of 69.0%and extended cycling stability with 99.8%capacity retention after 1000 *** proof of principle,an SNCC-based PIC is fabricated and tested,achieving 94.3Wh kg^(−1)at 237.5Wkg^(−1)and sustaining over 6000 cycles at 30 A g−1 with 84.5%*** internal structure of S and N codoped SNCC is based on highly dilated and defective graphene sheets arranged into nanometer-scale *** a baseline S-free carbon for comparison(termed NCC),the role of S doping and the resultant dilated structure was *** to galvanostatic intermittent titration technique and electrochemical impedance spectroscopy analyses,as well as COMSOL simulations,this structure promotes rapid solid-state diffusion of potassium ions and a solid electrolyte interphase that is stable during cycling.X-ray diffraction was used to probe the ion storage mechanisms in SNCC,establishing the role of reversible potassium intercalation and the presence of KC36,KC24,and KC8 phases at low voltages.

关键词： carbon manufacturing commercial carbon graphene potassium ion battery(KIP,PIB) potassium ion storage

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Harnessing the flatbandλ-Ti_(3)O_(5):A breakthrough in solar steam generation

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science China materials 2023年第11期66卷 4515-4516页

作者： Chuxin Lei Guihua Yu Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at AustinAustinTX 78712USA

As global population rises,accompanied by escalating environmental pollution and climate change,numerous countries find themselves grappling with an acute scarcity of natural freshwater resources^([1]).Seawater desalination presents a compelling solution to this looming crisis,especially considering the oceans are Earth’s largest water reservoir^([2]).

关键词： reservoir Earth breakthrough

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Efficient First-Principles Framework for Overdamped Phonon Dynamics and Anharmonic Electron-Phonon Coupling in Superionic materials

arXiv

引用

arXiv 2025年

作者： Wang, Yuxuan Zacharias, Marios Zhang, Xiao Pant, Nick Even, Jacky Poudeu, Pierre F.P. Kioupakis, Emmanouil Department of Materials Science and Engineering University of Michigan Ann ArborMI48109 United States Univ Rennes INSA Rennes CNRS Institut FOTON - UMR 6082 RennesF-35000 France Applied Physics Program University of Michigan Ann ArborMI48109 United States Oden Institute for Computational Engineering and Sciences The University of Texas at Austin AustinTX78712 United States

Relying on the anharmonic special displacement method, we introduce an ab initio quasistatic polymorphous framework to describe local disorder, anharmonicity, and electron-phonon coupling in superionic conductors. Using the example of cubic Cu2Se, we show that positional polymorphism yields extremely overdamped anharmonic vibrations while preserving transverse acoustic phonons, consistent with experiments. We also demonstrate well-defined electronic band structures with large band gap openings due to polymorphism of 1.0 eV and calculate anharmonic electron-phonon renormalization, yielding band gap narrowing with increasing temperature in agreement with previous measurements. Our approach opens the way for efficient ab initio electronic structure calculations in superionic crystals to elucidate their compelling high figure-of-merit. © 2025, CC BY-NC-ND.

关键词： Energy gap

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Advancing optothermal manipulation:decoupling temperature and flow fields in quasi-isothermal microscale streaming

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Light(science & Applications) 2023年第9期12卷 1713-1714页

作者： Youngsun Kim Yuebing Zheng Materials Science and Engineering Program and Texas Materials Institute The University of Texas at AustinAustinTX78712USA Walker Department of Mechanical Engineering The University of Texas at AustinAustinTX78712USA

By decoupling temperature and flow fields through symmetry-correlated laser scan sequences,ISO-FLUCS enables quasi-isothermal optofluidic microscale *** technique offers precise control over fluid manipulation while m... 详细信息

关键词： thermal isothermal flow

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