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1.
Adv Sci (Weinh) ; : e2402162, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38708715

RESUMO

High-performance soft magnetic materials are important for energy conservation and emission reduction. One challenge is achieving a combination of reliable temperature stability, high resistivity, high Curie temperature, and high saturation magnetization in a single material, which often comes at the expense of intrinsic coercivity-a typical trade-off in the family of soft magnetic materials with homogeneous microstructures. Herein, a nanostructured FeCoNiSiAl complex concentrated alloy is developed through a hierarchical structure strategy. This alloy exhibits superior soft magnetic properties up to 897 K, maintaining an ultra-low intrinsic coercivity (13.6 A m-1 at 297 K) over a wide temperature range, a high resistivity (138.08 µΩ cm-1 at 297 K) and the saturation magnetization with only a 16.7% attenuation at 897 K. These unusual property combinations are attributed to the dual-magnetic-state nature with exchange softening due to continuous crystal ordering fluctuations at the atomic scale. By deliberately controlling the microstructure, the comprehensive performance of the alloy can be tuned and controlled. The research provides valuable guidance for the development of soft magnetic materials for high-temperature applications and expands the potential applications of related functional materials in the field of sustainable energy.

2.
Nano Lett ; 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38743874

RESUMO

Accurately decoding the three-dimensional atomic structure of surface active sites is essential yet challenging for a rational catalyst design. Here, we used comprehensive techniques combining the pair distribution function and reverse Monte Carlo simulation to reveal the surficial distribution of Pd active sites and adjacent coordination environment in palladium-copper nanoalloys. After the fine-tuning of the atomic arrangement, excellent catalytic performance with 98% ethylene selectivity at complete acetylene conversion was obtained in the Pd34Cu66 nanocatalysts, outperforming most of the reported advanced catalysts. The quantitative deciphering shows a large number of active sites with a Pd-Pd coordination number of 3 distributed on the surface of Pd34Cu66 nanoalloys, which play a decisive role in highly efficient semihydrogenation. This finding not only opens the way for guiding the precise design of bimetal nanocatalysts from atomic-level insight but also provides a method to resolve the spatial structure of active sites.

3.
ACS Appl Mater Interfaces ; 16(15): 19094-19102, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38571376

RESUMO

Due to the spontaneous transport of small-sized cations and redox reactions under open circuit conditions, the currently reported coloring electrochromic devices (ECDs) may self-bleach easily. The resulting ECDs exhibit poor open-circuit memory, which limits their applications in static display advertisement. By constructing energy barriers to effectively control small-sized cation transport, the redox reaction could be suppressed, thereby inhibiting the self-bleaching of ECDs. In this study, phosphate glass is used as an electrolyte to construct high-energy barriers. Sodium ions in phosphate glass absorb external heat to cross energy barriers and become conductive charge carriers. In this case, the electrochromism of ECDs is allowed. On the contrary, after the absorbed heat energy is released, sodium ions are immediately trapped by oxygen ions in the PO4 unit, becoming frozen ions. At this point, the electrochromization of ECDs is prohibited. Based on the ionic conductive feature of phosphate glass, ECDs absorb heat and are colored by applying an electric field first. Then, ECDs release the thermal energy and the sodium ions transport in the electrolyte is blocked to cut off the self-bleaching pathway. The prepared inorganic all-solid-state ECDs maintained the colored state for several months using the method mentioned above, which solved the problem of the poor open-circuit memory of ECDs.

4.
Nat Commun ; 15(1): 2925, 2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38575649

RESUMO

The advancement of laser-induced graphene (LIG) technology has streamlined the fabrications of flexible graphene devices. However, the ultrafast kinetics triggered by laser irradiation generates intrinsic amorphous characteristics, leading to high resistivity and compromised performance in electronic devices. Healing graphene defects in specific patterns is technologically challenging by conventional methods. Herein, we report the rapid rectification of LIG's topological defects by flash Joule heating in milliseconds (referred to as F-LIG), whilst preserving its overall structure and porosity. The F-LIG exhibits a decreased ID/IG ratio from 0.84 - 0.33 and increased crystalline domain from Raman analysis, coupled with a 5-fold surge in conductivity. Pair distribution function and atomic-resolution imaging delineate a broader-range order of F-LIG with a shorter C-C bond of 1.425 Å. The improved crystallinity and conductivity of F-LIG with excellent flexibility enables its utilization in high-performance soft electronics and low-voltage disinfections. Notably, our F-LIG/polydimethylsiloxane strain sensor exhibits a gauge factor of 129.3 within 10% strain, which outperforms pristine LIG by 800%, showcasing significant potential for human-machine interfaces.

5.
Adv Sci (Weinh) ; : e2307397, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38650173

RESUMO

Li-rich Mn-based layered oxides (LLO) hold great promise as cathode materials for lithium-ion batteries (LIBs) due to their unique oxygen redox (OR) chemistry, which enables additional capacity. However, the LLOs face challenges related to the instability of their OR process due to the weak transition metal (TM)-oxygen bond, leading to oxygen loss and irreversible phase transition that results in severe capacity and voltage decay. Herein, a synergistic electronic regulation strategy of surface and interior structures to enhance oxygen stability is proposed. In the interior of the materials, the local electrons around TM and O atoms may be delocalized by surrounding Mo atoms, facilitating the formation of stronger TM─O bonds at high voltages. Besides, on the surface, the highly reactive O atoms with lone pairs of electrons are passivated by additional TM atoms, which provides a more stable TM─O framework. Hence, this strategy stabilizes the oxygen and hinders TM migration, which enhances the reversibility in structural evolution, leading to increased capacity and voltage retention. This work presents an efficient approach to enhance the performance of LLOs through surface-to-interior electronic structure modulation, while also contributing to a deeper understanding of their redox reaction.

6.
Nat Mater ; 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38605195

RESUMO

The strength-ductility trade-off has long been a Gordian knot in conventional metallic structural materials and it is no exception in multi-principal element alloys. In particular, at ultrahigh yield strengths, plastic instability, that is, necking, happens prematurely, because of which ductility almost entirely disappears. This is due to the growing difficulty in the production and accumulation of dislocations from the very beginning of tensile deformation that renders the conventional dislocation hardening insufficient. Here we propose that premature necking can be harnessed for work hardening in a VCoNi multi-principal element alloy. Lüders banding as an initial tensile response induces the ongoing localized necking at the band front to produce both triaxial stress and strain gradient, which enables the rapid multiplication of dislocations. This leads to forest dislocation hardening, plus extra work hardening due to the interaction of dislocations with the local-chemical-order regions. The dual work hardening combines to restrain and stabilize the premature necking in reverse as well as to facilitate uniform deformation. Consequently, a superior strength-and-ductility synergy is achieved with a ductility of ~20% and yield strength of 2 GPa during room-temperature and cryogenic deformation. These findings offer an instability-control paradigm for synergistic work hardening to conquer the strength-ductility paradox at ultrahigh yield strengths.

7.
Sci Rep ; 14(1): 8400, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38600140

RESUMO

Due to the increased frequency of extreme weather events and the implementation of the China's dual-carbon target, thermal power companies have been under pressure to construct green infrastructure and to actively pursue low-carbon transformation in response to stricter environmental regulations. This research thus selects 30 listed thermal power enterprises in China as study objects and assesses their green investment efficiency in the low-carbon transition process using three-stage DEA evaluation model with environmental regulation as an exogenous variable. Based on this, a benchmark regression model is used to corroborate the relationship between environmental regulation and green investment. Simultaneously, we carry out analysis to compare the correlation between thermal power firms' green investment efficiency and their focus on green investments. The results show in terms of total efficiency that environmental regulation significantly improves the total efficiency of 80% of thermal power enterprises compared to the absence of this exogenous variable. With the addition of environmental regulation, firms' total efficiency declines gradually in general from 2018 to 2022, with the mean value of efficiency falling by 0.068. In terms of stage-specific efficiency, the efficiency of the green investment stage of the majority of firms is between 0.3 and 0.6, which is much lower than that of the operational stage and the market performance stage. In terms of sub-indicator efficiency, both green investment efficiency and social donation efficiency among thermal power enterprises show obvious polarization, with 30% of them having an efficiency of 1 and 30% less than 0.1. In terms of green investment focus, thermal power unit renovation has a more obvious role in boosting the green investment efficiency of thermal power enterprises than do wind power and photovoltaic projects. Therefore, both governmental departments and thermal power enterprises need to take active measures in order to achieve green transformation from the perspective of green investment efficiency. Through the segmentation of important projects of green investment, this paper provides a reasonable investment direction reference for the sustainable transformation of China's thermal power industry. It also provides a rich and novel theoretical basis for the Chinese government to further improve the relevant environmental protection laws and regulations of thermal power industry.

8.
Small ; : e2401443, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38676339

RESUMO

The as-reported doping entropy engineering of electrode materials that are usually realized by the sharing of multiple metal elements with the metal element from the lattice body, potentially has three shortages of stringent synthesis conditions, large active element loss, and serious lattice distortion. Herein, an interlayer entropy engineering of layered oxide cathodes is proposed, where the multiple metal ions are simultaneously intercalated into the same interlayer sites, thus avoiding the three shortages. Concretely, a novel interlayer medium-entropy V2O5 ((MnCoNiMgZn)0.26V2O5∙0.84H2O) is successfully constructed by a one-step hydrothermal method. The interlayer medium-entropy effect is revealed to be that five metal ions pre-intercalation induces the local symmetry-broken [VO6] octahedra in bilayer V2O5, thus activating the reversible high-voltage redox reaction, inhibiting the layer slip and following phase transformation by its pinning effect, and enhancing the charge transfer kinetics. As a result, the medium-entropy cathode realizes the trade-off between specific capacity and structural stability with a discharge capacity of 152 mAh g-1 at 0.1 A g-1 after 100 cycles, and a capacity retention rate of 98.7% at 0.5 A g-1 after 150 cycles for Li+ storage. This engineering provides a new guideline for the rational design of high-performance layered oxide cathodes.

9.
Natl Sci Rev ; 11(4): nwae026, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38405434

RESUMO

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering (LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys (RHEAs). In contrast to conventional 'trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength (1160 MPa) and uniform ductility (24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

10.
Nature ; 625(7996): 697-702, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38172639

RESUMO

Body-centred cubic refractory multi-principal element alloys (MPEAs), with several refractory metal elements as constituents and featuring a yield strength greater than one gigapascal, are promising materials to meet the demands of aggressive structural applications1-6. Their low-to-no tensile ductility at room temperature, however, limits their processability and scaled-up application7-10. Here we present a HfNbTiVAl10 alloy that shows remarkable tensile ductility (roughly 20%) and ultrahigh yield strength (roughly 1,390 megapascals). Notably, these are among the best synergies compared with other related alloys. Such superb synergies derive from the addition of aluminium to the HfNbTiV alloy, resulting in a negative mixing enthalpy solid solution, which promotes strength and favours the formation of hierarchical chemical fluctuations (HCFs). The HCFs span many length scales, ranging from submicrometre to atomic scale, and create a high density of diffusive boundaries that act as effective barriers for dislocation motion. Consequently, versatile dislocation configurations are sequentially stimulated, enabling the alloy to accommodate plastic deformation while fostering substantial interactions that give rise to two unusual strain-hardening rate upturns. Thus, plastic instability is significantly delayed, which expands the plastic regime as ultralarge tensile ductility. This study provides valuable insights into achieving a synergistic combination of ultrahigh strength and large tensile ductility in MPEAs.

11.
Chaos ; 34(1)2024 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-38198679

RESUMO

We study the effect of relative phase on the characteristics of rogue waves and solitons described by rational solutions in the nonlinear Schrödinger Maxwell-Bloch system. We derived the rational rogue wave and soliton solutions with adjustable relative phase and present the parameter range of different types of rogue waves and solitons. Our findings show that the relative phase can alter the distribution of rational solitons and even change the type of rational solitons, leading to a rich array of rational soliton types by adjusting the relative phase. However, the relative phase does not affect the structure of the rogue wave, because the relative phase of the rogue wave changes during evolution. In particular, we confirm that the rational solitons with varying relative phases and the rogue waves at corresponding different evolution positions share the same distribution mode. This relationship holds true for rogue waves or breathers and their stable counterparts solitons or periodic waves in different nonlinear systems. The implications of our study are significant for exploring fundamental excitation elements in nonlinear systems.

13.
Adv Mater ; 36(13): e2302647, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37993111

RESUMO

All-solid-state lithium metal batteries can address crucial challenges regarding insufficient battery cycling life and energy density. The demonstration of long-cycling dendrite-free all-solid-state lithium metal batteries requires precise tailoring of lithium-ion transport of solid-state electrolytes (SSEs). In this work, a proof of concept is reported for precise tailoring of lithium-ion transport of a halide SSE, Li3InCl6, including intragranular (within grains) but also intergranular (between grains) lithium-ion transport. Lithium-ion migration tailoring mechanism in crystals is developed by unexpected enhanced Li, In, and Cl vacancy populations and lower energy barrier for hopping. The lithium-ion transport tailoring mechanism between the grains is determined by the elimination of voids between grains and the formation of unexpected supersonic conducting grain boundaries, boosting the lithium dendrite suppression ability of SSE. Due to boosted lithium-ion conduction and dendrite-suppression ability, the all-solid-state lithium metal batteries coupled with Ni-rich LiNi0.83Co0.12Mn0.05O2 cathodes and lithium metal anodes demonstrate breakthroughs in electrochemical performance by achieving extremely long cycling life at a high current density of 0.5 C (2000 cycles, 93.7% capacity retention). This concept of precise tailoring of lithium-ion transport provides a cost, time, and energy efficient solution to conquer the remaining challenges in all-solid-state lithium-metal batteries for fast developing electric vehicle markets.

14.
Waste Manag ; 174: 320-327, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38091656

RESUMO

Disposal of automobile shredder residue (ASR) via pyrolysis enables the recovery of valuable products; however, the production of hazardous pollutants and low-value products is inevitable due to its high chlorine content. In this work, chlorine evolution behavior and the conversion mechanism during ASR pyrolysis between 480 and 600 °C were systematically studied. The experimental results for organic chlorine (Org-Cl) showed that released chlorinated gases were complex, and HCl only accounted for 35% of the gas phase products, while short-chain hydrocarbons with carbon atoms between two and four accounted for 52%. Chlorine was predominantly retained in the char, and Org-Cl was the primary contributor to the residual chlorine, accounting for over 50% of the char. The content of inorganic chlorine (InO-Cl) was low in the raw sample but significantly increased in the char. Through the distinction between organic and inorganic chlorine content in char, it was confirmed that Org-Cl could be converted to InO-Cl due to complex secondary reactions with metallic compounds. The conversion was favored by increasing the Org-Cl content and the temperature. Our findings clarified the evolution mechanism of chlorine and the transformation from Org-Cl to InO-Cl, thus providing guidance for chlorine regulation and the efficient recycling of metal resources.


Assuntos
Automóveis , Cloro , Pirólise , Reciclagem , Metais , Gases/química
15.
Small ; 20(16): e2307792, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38037483

RESUMO

A high-throughput ion beam sputtering system is used to synthesize compositional gradient superlattice-like (SLL) thin film libraries of Ge-Sb-Te alloys over the entire phase diagram. The optical properties and structural evolution of the Ge-Sb-Te combinatorial SLL thin film are investigated. A systematic screening over the annealing temperature, annealing time, and modulation period has elucidated the critical factors that affect the stability of the metastable phase and optical properties. It is found that amorphous stability and optical constant are highly dependent on the modulation period and chemical composition of the thin film. This data-driven approach offers new perspectives for accelerating the development of new materials with excellent optical and amorphous stability and for exploring their mechanisms, by greatly expanding the dataset of Ge-Sb-Te alloys with SLL structures through high-throughput experiments.

16.
Virus Genes ; 60(1): 9-17, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37938470

RESUMO

Most wild strains of Japanese encephalitis virus (JEV) produce NS1' protein, which plays an important role in viral infection and immune escape. The G66A nucleotide mutation in NS2A gene of the wild strain SA14 prevented the ribosomal frameshift that prevented the production of NS1' protein, thus reduced the virulence. In this study, the 66th nucleotide of the NS2A gene of SA14 was mutated into A, U or C, respectively. Both the G66U and G66C mutations cause the E22D mutation of the NS2A protein. Subsequently, the expression of NS1' protein, plaque size, replication ability, and virulence to mice of the three mutant strains were examined. The results showed that the three mutant viruses could not express NS1' protein, and their proliferation ability in nerve cells and virulence to mice were significantly reduced. In addition, the SA14(G66C) was less virulent than the other two mutated viruses. Our results indicate that only when G is the 66th nucleotide of NS2A, the JEV can produce NS1' protein, which affects the virulence.


Assuntos
Vírus da Encefalite Japonesa (Espécie) , Encefalite Japonesa , Animais , Camundongos , Vírus da Encefalite Japonesa (Espécie)/genética , Nucleotídeos/metabolismo , Virulência/genética , Linhagem Celular , Proteínas não Estruturais Virais/metabolismo , Proliferação de Células
17.
Langmuir ; 40(1): 348-361, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38154090

RESUMO

In this study, hollow and hierarchical CuO micro-nano cubes wrapped by reduced graphene oxide (H-CuO MNCs@rGO) were designed and successfully fabricated via a novel three-step wet-chemical method. Benefiting from its unique hollow and hierarchical micro-nano structures, H-CuO MNCs@rGO exhibited significantly enhanced electrochemical Na+ storage performance when utilized as anode material for sodium-ion batteries (SIBs). Specifically, H-CuO MNCs@rGO demonstrated a specific capacity of 380.9 mAh g-1 in the initial reversible cycle and a capacity retention of 218.9 mAh g-1 after 150 cycles at a current density of 300 mA g-1. Furthermore, through the dominant pseudocapacitive behavior, an optimized rate capability of 221.2 mAh g-1 at 800 mA g-1 can be obtained for H-CuO MNCs@rGO. The comprehensive Na+ storage properties of H-CuO MNCs@rGO obviously exceeded those of hollow CuO cubes (H-CuO MNCs) and bulk CuO anodes. Such enhanced Na+ storage performances of H-CuO MNCs@rGO can be attributed to its reasonable hollow and hierarchical micro-nano structures, which provide abundant redox active sites, shorten Na+ migration pathway, buffer volume expansion, and improve electronic/ionic conductivity during sodiation/desodiation process. Our strategy provides a facile and innovative approach for the design of CuO with rational micro-nano structure as a high-performance anode for SIBs, which would also be a guiding way for tailoring transition metal oxides in other scalable and functional applications.

18.
J Am Chem Soc ; 145(49): 26728-26735, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-38015199

RESUMO

Deciphering the three-dimensional (3D) insight into nanocatalyst surfaces at the atomic level is crucial to understanding catalytic reaction mechanisms and developing high-performance catalysts. Nevertheless, better understanding the inherent insufficiency of a long-range ordered lattice in nanocatalysts is a big challenge. In this work, we report the local structure of Pd nanocatalysts, which is beneficial for demonstrating the shape-structure-adsorption relationship in acetylene hydrogenation. The 5.27 nm spherical Pd catalyst (Pdsph) shows an ethylene selectivity of 88% at complete acetylene conversion, which is much higher than those of the Pd octahedron and Pd cube and superior to other reported monometallic Pd nanocatalysts so far. By virtue of the local structure revelation combined with the atomic pair distribution function (PDF) and reverse Monte Carlo (RMC) simulation, the atomic surface distribution of the unique compressed strain of Pd-Pd pairs in Pdsph was revealed. Density functional theory calculations verified the obvious weakening of the ethylene adsorption energy on account of the surface strain of Pdsph. It is the main factor to avoid the over-hydrogenation of acetylene. The present work, entailing shape-induced surface strain manipulation and atomic 3D insight, opens a new path to understand and optimize chemical activity and selectivity in the heterogeneous catalysis process.

19.
Chem Commun (Camb) ; 59(94): 13982-13985, 2023 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-37937427

RESUMO

Lithium oxalate (Li2C2O4) is an attractive cathode pre-lithiation additive for lithium-ion batteries (LIBs), but its application is hindered by its high decomposition potential (>4.7 V). Due to the liquid-solid synergistic effect of the NaNO2 additive and the LiNi0.83Co0.07Mn0.1O2 (NCM) cathode material, the decomposition efficiency of micro-Li2C2O4 reaches 100% at a low charge cutoff voltage of 4.3 V. Our work boosts the widespread practical application of Li2C2O4 by a simple and promising electrolyte-assisted cathode pre-lithiation strategy.

20.
Materials (Basel) ; 16(19)2023 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-37834727

RESUMO

Ni-Mn-based Heusler alloys are known to demonstrate magnetic shape memory and giant magnetocaloric effect (MCE). These effects depend on the phases, crystallographic and magnetic phase transitions, and the crystallographic texture characteristics. These structural characteristics, in turn, are a function of the processing parameters. In the current work, Ni55.5Mn18.8Ga24Si1.7 Heusler alloy was processed by melt-spinning under a helium atmosphere. This process results in a fine microstructure. The ribbon that was produced with a narrower nozzle width, faster wheel speed, and higher cast temperature, indicating a faster cooling rate, had double the magnetic entropy change close to room temperature. However, the other ribbon demonstrated a large entropy change over a broader temperature range, extending its usability. The effect of the melt-spinning process parameters on the developing microstructure, crystallographic structure and texture, transformation temperatures, and the magnetic entropy change were studied to explain the difference in magnetocaloric behavior.

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