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1.
In the present work, h‐RFeO3 multiferroic ceramics are designed and created by introducing chemical pressure (In‐substitution for Lu) in LuFeO3. Lu1?xInxFeO3 (x = 0‐0.75) ceramics are prepared by the standard solid‐state reaction process. The crystal structure of the present ceramics is tuned from centrosymmetric Pbnm (x = 0) to non‐centrosymmetric P63cm (x = 0.4–0.6), and subsequently to centrosymmetric P63/mmc (x = 0.75), while the Pbnm and P63cm biphase structure is detected for x = 0.25. The Curie temperature for the polar P63cm (x = 0.4–0.6) phase decreases from >1000 to ≈550 K with increasing x. Cloverleaf ferroelectric domain structures are determined in polar Lu0.5In0.5FeO3 samples, and the ferroelectric domain walls at atomic scale are evaluated by the aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy (HAADF STEM), where the spontaneous polarization of 1.73 µC cm?2 is determined for x = 0.5. The spontaneous polarization is also confirmed by calculating the site displacement from the centrosymmetric phase based on the X‐ray diffraction (XRD) data. Meanwhile, two magnetic transitions are determined for all compositions, that is, paramagnetic to antiferromagnetic transition at Néel temperature TN (≈350 K for x = 0.4–0.6), and antiferromagnetic to weak‐ferromagnetic transition at spin‐reorientation temperature TSR. The co‐presence of ferroelectric and antiferromagnetic orders confirms the present ceramics as promising room‐temperature multiferroic materials.  相似文献   

2.
Li‐ion batteries containing cost‐effective, environmentally benign cathode materials with high specific capacities are in critical demand to deliver the energy density requirements of electric vehicles and next‐generation electronic devices. Here, the phase‐controlled synthesis of copper sulfide (CuxS) composites by the temperature‐controlled sulfurization of a prototypal Cu metal‐organic framework (MOF), HKUST‐1 is reported. The tunable formation of different CuxS phases within a carbon network represents a simple method for the production of effective composite cathode materials for Li‐ion batteries. A direct link between the sulfurization temperature of the MOF and the resultant CuxS phase formed with more Cu‐rich phases favored at higher temperatures is further shown. The CuxS/C samples are characterized through X‐ray diffraction (XRD), thermogravimetric analysis (TGA), transmission electron microscopy, and energy dispersive X‐ray spectroscopy (EDX) in addition to testing as Li‐ion cathodes. It is shown that the performance is dependent on both the CuxS phase and the crystal morphology with the Cu1.8S/C‐500 material as a nanowire composite exhibiting the best performance, showing a specific capacity of 220 mAh g?1 after 200 charge/discharge cycles.  相似文献   

3.
The rational combination of conductive nanocarbon with sulfur leads to the formation of composite cathodes that can take full advantage of each building block; this is an effective way to construct cathode materials for lithium–sulfur (Li–S) batteries with high energy density. Generally, the areal sulfur‐loading amount is less than 2.0 mg cm?2, resulting in a low areal capacity far below the acceptable value for practical applications. In this contribution, a hierarchical free‐standing carbon nanotube (CNT)‐S paper electrode with an ultrahigh sulfur‐loading of 6.3 mg cm?2 is fabricated using a facile bottom–up strategy. In the CNT–S paper electrode, short multi‐walled CNTs are employed as the short‐range electrical conductive framework for sulfur accommodation, while the super‐long CNTs serve as both the long‐range conductive network and the intercrossed mechanical scaffold. An initial discharge capacity of 6.2 mA·h cm?2 (995 mA·h g?1), a 60% utilization of sulfur, and a slow cyclic fading rate of 0.20%/cycle within the initial 150 cycles at a low current density of 0.05 C are achieved. The areal capacity can be further increased to 15.1 mA·h cm?2 by stacking three CNT–S paper electrodes—resulting in an areal sulfur‐loading of 17.3 mg cm?2—for the cathode of a Li–S cell. The as‐obtained free‐standing paper electrode are of low cost and provide high energy density, making them promising for flexible electronic devices based on Li–S batteries.  相似文献   

4.
In this work, a full‐cell sodium‐ion battery (SIB) with a high specific energy approaching 300 Wh kg?1 is realized using a sodium vanadium fluorophosphate (Na3V2(PO4)2F3, NVPF) cathode and a tin phosphide (SnPx) anode, despite both electrode materials having greatly unbalanced specific capacities. The use of a cathode employing an areal loading more than eight times larger than that of the anode can be achieved by designing a nanostructured nanosized NVPF (n‐NVPF) cathode with well‐defined particle size, porosity, and conductivity. Furthermore, the high rate capability and high potential window of the full‐cell can be obtained by tuning the Sn/P ratio (4/3, 1/1, and 1/2) and the nanostructure of an SnPx/carbon composite anode. As a result, the full‐cell SIBs employing the nanostructured n‐NVPF cathode and the SnPx/carbon composite anode (Sn/P = 1/1) exhibit outstanding specific energy (≈280 Wh kg?1(cathode+anode)) and energy efficiency (≈78%); furthermore, the results are comparable to those of state‐of‐the‐art lithium‐ion batteries.  相似文献   

5.
Solution‐processed metal‐oxide thin films based on high dielectric constant (k) materials have been extensively studied for use in low‐cost and high‐performance thin‐film transistors (TFTs). Here, scandium oxide (ScOx) is fabricated as a TFT dielectric with excellent electrical properties using a novel water‐inducement method. The thin films are annealed at various temperatures and characterized by using X‐ray diffraction, atomic‐force microscopy, X‐ray photoelectron spectroscopy, optical spectroscopy, and a series of electrical measurements. The optimized ScOx thin film exhibits a low‐leakage current density of 0.2 nA cm?2 at 2 MV cm?1, a large areal capacitance of 460 nF cm?2 at 20 Hz and a permittivity of 12.1. To verify the possible applications of ScOx thin films as the gate dielectric in complementary metal oxide semiconductor (CMOS) electronics, they were integrated in both n‐type InZnO (IZO) and p‐type CuO TFTs for testing. The water‐induced full oxide IZO/ScOx TFTs exhibit an excellent performance, including a high electron mobility of 27.7 cm2 V?1 s?1, a large current ratio (Ion/Ioff) of 2.7 × 107 and high stability. Moreover, as far as we know it is the first time that solution‐processed p‐type oxide TFTs based on a high‐k dielectric are achieved. The as‐fabricated p‐type CuO/ScOx TFTs exhibit a large Ion/Ioff of around 105 and a hole mobility of 0.8 cm2 V?1 at an operating voltage of 3 V. To the best of our knowledge, these electrical parameters are among the highest performances for solution‐processed p‐type TFTs, which represents a great step towards the achievement of low‐cost, all‐oxide, and low‐power consumption CMOS logics.  相似文献   

6.
Lithium–sulfur battery is recognized as one of the most promising energy storage devices, while the application and commercialization are severely hindered by both the practical gravimetric and volumetric energy densities due to the low sulfur content and tap density with lightweight and nonpolar porous carbon materials as sulfur host. Herein, for the first time, conductive CoOOH sheets are introduced as carbon‐free sulfur immobilizer to fabricate sulfur‐based composite as cathode for lithium–sulfur battery. CoOOH sheet is not only a good sulfur‐loading matrix with high electron conductivity, but also exhibits outstanding electrocatalytic activity for the conversion of soluble lithium polysulfide. With an ultrahigh sulfur content of 91.8 wt% and a tap density of 1.26 g cm?3, the sulfur/CoOOH composite delivers high gravimetric capacity and volumetric capacity of 1199.4 mAh g?1‐composite and 1511.3 mAh cm?3 at 0.1C rate, respectively. Meanwhile, the sulfur‐based composite presents satisfactory cycle stability with a slow capacity decay rate of 0.09% per cycle within 500 cycles at 1C rate, thanks to the strong interaction between CoOOH and soluble polysulfides. This work provides a new strategy to realize the combination of gravimetric energy density, volumetric energy density, and good electrochemical performance of lithium–sulfur battery.  相似文献   

7.
Rechargeable aqueous Zn‐based batteries, benefiting from their good reliability, low cost, high energy/power densities, and ecofriendliness, show great potential in energy storage systems. However, the poor cycling performance due to the formation of Zn dendrites greatly hinders their practical applications. In this work, a trilayer 3D CC‐ZnO@C‐Zn anode is obtained by in situ growing ZIFs (zeolitic‐imidazolate frameworks) derived ZnO@C core–shell nanorods on carbon cloth followed by Zn deposition, which exhibits excellent antidendrite performance. Using CC‐ZnO@C‐Zn as the anode and a branch‐like Co(CO3)0.5(OH)x·0.11H2O@CoMoO4 (CC‐CCH@CMO) as the cathode, a Zn–Co battery is rationally designed, displaying excellent energy/power densities (235 Wh kg?1, 12.6 kW kg?1) and remarkable cycling performance (71.1% after 5000 cycles). Impressively, when using a gel electrolyte, a highly customizable, fiber‐shaped flexible all‐solid‐state Zn–Co battery is assembled for the first time, which presents a high energy density of 4.6 mWh cm?3, peak power density of 0.42 W cm?3, and long durability (82% capacity retention after 1600 cycles) as well as excellent flexibility. The unique 3D electrode design in this study provides a novel approach to achieve high‐performance Zn‐based batteries, showing promising applications in flexible and portable energy‐storage systems.  相似文献   

8.
Nitrogen‐rich porous carbons (NPCs) are the leading cathode materials for next‐generation Zn–air and Li–S batteries. However, most existing NPC suffers from insufficient exposure and harnessing of nitrogen‐dopants (NDs), constraining the electrochemical performance. Herein, by combining silica templating with in situ texturing of metal–organic frameworks, a new bifunctional 3D nitrogen‐rich carbon photonic crystal architecture of simultaneously record‐high total pore volume (13.42 cm3 g?1), ultralarge surface area (2546 m2 g?1), and permeable hierarchical macro‐meso‐microporosity is designed, enabling sufficient exposure and accessibility of NDs. Thus, when used as cathode catalysts, the Zn–air battery delivers a fantastic capacity of 770 mAh gZn?1 at an unprecedentedly high rate of 120 mA cm?2, with an ultrahigh power density of 197 mW cm?2. When hosting 78 wt% sulfur, the Li–S battery affords a high‐rate capacity of 967 mAh g?1 at 2 C, with superb stability over 1000 cycles at 0.5 C (0.054% decay rate per cycle), comparable to the best literature value. The results prove the dominant role of highly exposed graphitic‐N in boosting both cathode performances.  相似文献   

9.
Transparent p‐type semiconductors with wide‐range tunability of the hole density are rare. Developing such materials is a challenge in the field of transparent electronics that utilize invisible electric circuits. In this paper, a CuI–CuBr alloy (CuI1?xBrx) is proposed as a hole‐density‐tunable p‐type transparent semiconductor that can be fabricated at room temperature. First‐principles calculations predict that the acceptor state originating from copper vacancies in CuBr is deeper than that in CuI, leading to the hypothesis that the hole density in CuI1?xBrx can be tuned over a wide range by varying x between 0 and 1. The experimental results support this hypothesis. The hole density in CuI1?xBrx polycrystalline alloy layers can be tuned by over three orders of magnitude (1017–1020 cm?3) by varying x. In other words, the p‐type conductivity of the CuI1?xBrx alloy shows metallic and semiconducting properties. Such alloy layers can be prepared at room temperature without sacrificing transparency. Furthermore, CuI1?xBrx forms transparent p–n diodes with n‐type amorphous In–Ga–Zn–O layers, and these diodes have satisfactory rectification performance. Therefore, CuI1?xBrx alloy is an excellent p‐type transparent semiconductor for which the p‐type conductivity can be tailored in a wide range.  相似文献   

10.
Highly efficient non‐noble metal electrocatalysts are vital for metal–air batteries and fuel cells. Herein, a noble‐metal–free single‐atom Fe‐N x‐C electrocatalyst is synthesized by incorporating Fe‐Phen complexes into the nanocages in situ during the growth of ZIF‐8, followed by pyrolysis at 900 °C under inert atmosphere. Fe‐Phen species provide both Fe2+ and the organic ligand (Phen) simultaneously, which play significant roles in preparing single‐atom catalysts. The obtained Fe‐Nx‐C exhibits a half‐wave potential of 0.91 V for the oxygen reduction reaction, higher than that of commercial Pt/C (0.82 V). As a cathode catalyst for primary zinc–air batteries (ZABs), the battery shows excellent electrochemical performances in terms of the high open‐circuit voltage (OCV) of 1.51 V and a high power density of 96.4 mW cm?2. The rechargeable ZAB with Fe‐Nx‐C catalyst and the alkaline electrolyte shows a remarkable cycling performance for 300 h with an initial round‐trip efficiency of 59.6%. Furthermore, the rechargeable all‐solid‐state ZABs with the Fe‐Nx‐C catalyst show high OCV of 1.49 V, long cycle life for 120 h, and foldability. The single‐atom Fe‐Nx‐C electrocatalyst may function as a promising catalyst for various metal–air batteries and fuel cells.  相似文献   

11.
In 2009, Karimi et al. reported that Bi1‐xNdxFeO3 0.15 ≤ x ≤ 0.25 exhibited a PbZrO3 (PZ)‐like structure. These authors presented some preliminary electrical data for the PZ‐like composition but noted that the conductivity was too high to obtain radio‐frequency measurements representative of the intrinsic properties. In this study, Bi0.85Nd0.15Fe1‐yTiyO3 (0 ≤ y ≤ 0.1) were investigated, in which Ti acted as a donor dopant on the B‐site. In contrast to the original study of Karimi et al., X‐ray diffraction (XRD) of Bi0.85Nd0.15FeO3 revealed peaks which were attributed to a mixture of PZ‐like and rhombohedral structures. However, as the Ti (0 < y ≤ 0.05) concentration increased, the rhombohedral peaks disappeared and all intensities were attributed to the PZ‐like phase. For y = 0.1, broad XRD peaks indicated a significant decrease in effective diffracting volume. Electron diffraction confirmed that the PZ‐like phase was dominant for y ≤ 0.05, but for y = 0.1, an incommensurate structure was present, consistent with the broadened XRD peaks. The substitution of Fe3+ by Ti4+ decreased the dielectric loss at room temperature from >0.3 to <0.04 for all doped compositions, with a minimum (0.015) observed for y = 0.03. The decrease in dielectric loss was accompanied by a decrease in the room temperature bulk conductivity from ~1 mS cm?1 to <1 μS cm?1 and an increase in bulk activation energy from 0.29 to >1 eV. Plots of permittivity (?r) versus temperature for 0.01 ≤ y ≤ 0.05 revealed a step rather than a peak in ?r on heating at the same temperature determined for the antiferroelectric–paraelectric phase transition by differential scanning calorimetry. Finally, large electric fields were applied to all doped samples which resulted in a linear dependence of polarisation on the electric field similar to that obtained for PbZrO3 ceramics under equivalent experimental conditions.  相似文献   

12.
Manganese phosphorus trichalcogenides are widely used in the field of photocatalysis and magnetic studies due to their broadband gaps. Herein, an alloy engineering method for the few‐layer manganese phosphorus trichalcogenides (MnPS3–xSex, 0 ≤ x ≤ 3) in surface‐enhanced Raman scattering (SERS) is reported. A new strategy, with the coupling of exciton resonance (µex) and photoinduced charge transfer (PICT), is applied to screen out materials for SERS enhancement. According to the calculation of density functional theory, the bandgap of manganese phosphorus trichalcogenides (MnPS3) can be adjusted to match the band energy of Rhodamine 6G molecules by alloy engineering. Furthermore, a series of few‐layer MnPS3–xSex (0 ≤ x ≤ 3) are fabricated to study the PICT‐induced SERS behavior under resonance excitation. The good performance with a detection limit down to 10?9 m indicates that the synergistic resonances between µex and PICT are crucial to the enhancement.  相似文献   

13.
Making highly efficient catalysts for an overall ?water splitting reaction is vitally important to bring solar/electrical‐to‐hydrogen energy conversion processes into reality. Herein, the synthesis of ultrathin nanosheet‐based, hollow MoOx/Ni3S2 composite microsphere catalysts on nickel foam, using ammonium molybdate as a precursor and the triblock copolymer pluronic P123 as a structure‐directing agent is reported. It is also shown that the resulting materials can serve as bifunctional, non‐noble metal electrocatalysts with high activity and stability for the hydrogen evolution reaction (HER) as well as the oxygen evolution reaction (OER). Thanks to their unique structural features, the materials give an impressive water‐splitting current density of 10 mA cm?2 at ≈1.45 V with remarkable durability for >100 h when used as catalysts both at the cathode and the anode sides of an alkaline electrolyzer. This performance for an overall water splitting reaction is better than even those obtained with an electrolyzer consisting of noble metal‐based Pt/C and IrOx/C catalytic couple—the benchmark catalysts for HER and OER, respectively.  相似文献   

14.
The construction of a novel 3D self‐supported integrated NixCo2?xP@NC (0 < x < 2) nanowall array (NA) on Ni foam (NF) electrode constituting highly dispersed NixCo2?xP nanoparticles, nanorods, nanocapsules, and nanodendrites embedded in N‐doped carbon (NC) NA grown on NF is reported. Benefiting from the collective effects of special morphological and structural design and electronic structure engineering, the NixCo2?xP@NC NA/NF electrodes exhibit superior electrocatalytic performance for water splitting with an excellent stability in a wide pH range. The optimal NiCoP@NC NA/NF electrode exhibits the best hydrogen evolution reaction (HER) activity in acidic solution so far, attaining a current density of 10 mA cm?2 at an overpotential of 34 mV. Moreover, the electrode manifests remarkable performances toward both HER and oxygen evolution reaction in alkaline medium with only small overpotentials of 37 mV at 10 mA cm?2 and 305 mV at 50 mA cm?2, respectively. Most importantly, when coupling with the NiCoP@NC NA/NF electrode for overall water splitting, an alkali electrolyzer delivers a current density of 20 mA cm?2 at a very low cell voltage of ≈1.56 V. In addition, the NiCoP@NC NA/NF electrode has outstanding long‐term durability at j = 10 mA cm?2 with a negligible degradation in current density over 22 h in both acidic and alkaline media.  相似文献   

15.
Room‐temperature Na‐ion batteries (NIBs) have recently attracted attention as potential alternatives to current Li‐ion batteries (LIBs). The natural abundance of sodium and the similarity between the electrochemical properties of NIBs and LIBs make NIBs well suited for applications requiring low cost and long‐term reliability. Here, the first successful synthesis of a series of Na3(VO1?x PO4)2F1+2x (0 ≤ x ≤ 1) compounds as a new family of high‐performance cathode materials for NIBs is reported. The Na3(VO1?x PO4)2F1+2x series can function as high‐performance cathodes for NIBs with high energy density and good cycle life, although the redox mechanism varies depending on the composition. The combined first‐principles calculations and experimental analysis reveal the detailed structural and electrochemical mechanisms of the various compositions in solid solutions of Na3(VOPO4)2F and Na3V2(PO4)2F3. The comparative data for the Na y (VO1?x PO4)2F1+2x electrodes show a clear relationship among V3+/V4+/V5+ redox reactions, Na+?Na+ interactions, and Na+ intercalation mechanisms in NIBs. The new family of high‐energy cathode materials reported here is expected to spur the development of low‐cost, high‐performance NIBs.  相似文献   

16.
Practical electrochemical water splitting requires cost‐effective electrodes capable of steadily working at high output, leading to the challenges for efficient and stable electrodes for the oxygen evolution reaction (OER). Herein, by simply using conductive FeS microsheet arrays vertically pre‐grown on iron foam (FeS/IF) as both substrate and source to in situ form vertically aligned NiFe(OH)x nanosheets arrays, a hierarchical electrode with a nano/micro sheet‐on‐sheet structure (NiFe(OH)x/FeS/IF) can be readily achieved to meet the requirements. Such hierarchical electrode architecture with a superhydrophilic surface also allows for prompt gas release even at high output. As a result, NiFe(OH)x/FeS/IF exhibits superior OER activity with an overpotential of 245 mV at 50 mA cm?2 and can steadily output 1000 mA cm?2 at a low overpotential of 332 mV. The water‐alkali electrolyzer using NiFe(OH)x/FeS/IF as the anode can deliver 10 mA cm?2 at 1.50 V and steadily operate at 300 mA cm?2 with a small cell voltage for 70 h. Furthermore, a solar‐driven electrolyzer using the developed electrode demonstrates an exceptionally high solar‐to‐hydrogen efficiency of 18.6%. Such performance together with low‐cost Fe‐based materials and facile mass production suggest the present strategy may open up opportunities for rationally designing hierarchical electrocatalysts for practical water splitting or diverse applications.  相似文献   

17.
Rather than using three layers, including an electrolyte, a working fuel cell is created that employs only one homogenous layer with mixed conductivity. The layer is a composite made from a mixture of metal oxide, Li0.15Ni0.45Zn0.4 oxide, and an ionic conductor; ion‐doped ceria. The single‐component layer has a total conductivity of 0.1–1 S cm?1 and exhibits both ionic and semiconducting properties. This homogenous one‐layer device has a power output of more than 600 mW cm?2 at 550 °C operating with H2 and air. Overall conversion is completed in a similar way to a traditional fuel cell, even though the device does not include the electrolyte layer critical for traditional fuel‐cell technologies using the three‐component anode–electrolyte–cathode structure.  相似文献   

18.
Additive patterning of transparent conducting metal oxides at low temperatures is a critical step in realizing low‐cost transparent electronics for display technology and photovoltaics. In this work, inkjet‐printed metal oxide transistors based on pure aqueous chemistries are presented. These inks readily convert to functional thin films at lower processing temperatures (T ≤ 250 °C) relative to organic solvent‐based oxide inks, facilitating the fabrication of high‐performance transistors with both inkjet‐printed transparent electrodes of aluminum‐doped cadmium oxide (ACO) and semiconductor (InOx ). The intrinsic fluid properties of these water‐based solutions enable the printing of fine features with coffee‐ring free line profiles and smoother line edges than those formed from organic solvent‐based inks. The influence of low‐temperature annealing on the optical, electrical, and crystallographic properties of the ACO electrodes is investigated, as well as the role of aluminum doping in improving these properties. Finally, the all‐aqueous‐printed thin film transistors (TFTs) with inkjet‐patterned semiconductor (InOx ) and source/drain (ACO) layers are characterized, which show ideal low contact resistance (R c < 160 Ω cm) and competitive transistor performance (µ lin up to 19 cm2 V?1 s?1, Subthreshold Slope (SS) ≤150 mV dec?1) with only low‐temperature processing (T ≤ 250 °C).  相似文献   

19.
Efficient hydrogen evolution reaction (HER) over noble‐metal‐free electrocatalysts provides one of the most promising pathways to face the energy crisis. Herein, facile cobalt‐doping based on Co‐modified MoOx–amine precursors is developed to optimize the electrochemical HER over Mo2C nanowires. The effective Co‐doping into Mo2C crystal structure increases the electron density around Fermi level, resulting in the reduced strength of Mo–H for facilitated HER kinetics. As expected, the Co‐Mo2C nanowires with an optimal Co/Mo ratio of 0.020 display a low overpotential (η10 = 140 and 118 mV for reaching a current density of –10 mA cm?2; η100 = 200 and 195 mV for reaching a current density of –100 mA cm?2), a small Tafel slope (39 and 44 mV dec?1), and a low onset overpotential (40 and 25 mV) in 0.5 m H2SO4 and 1.0 m KOH, respectively. This work highlights a feasible strategy to explore efficient electrocatalysts via engineering on composition and nanostructure.  相似文献   

20.
A self‐assembled GeOx/reduced graphene oxide (GeOx/RGO) composite, where GeOx nanoparticles are grown directly on reduced graphene oxide sheets, is synthesized via a facile one‐step reduction approach and studied by X‐ray diffraction, transmission electron microscopy, energy dispersive X‐ray spectroscopy, electron energy loss spectroscopy elemental mapping, and other techniques. Electrochemical evaluation indicates that incorporation of reduced graphene oxide enhances both the rate capability and reversible capacity of GeOx, with the latter being due to the RGO enabling reversible utilization of Li2O. The composite delivers a high reversible capacity of 1600 mAh g?1 at a current density of 100 mA g?1, and still maintains a capacity of 410 mAh g?1 at a high current density of 20 A g?1. Owing to the flexible reduced graphene oxide sheets enwrapping the GeOx particles, the cycling stability of the composite is also improved significantly. To further demonstrate its feasibility in practical applications, the synthesized GeOx/RGO composite anode is successfully paired with a high voltage LiNi0.5Mn1.5O4 cathode to form a full cell, which shows good cycling and rate performance.  相似文献   

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