Large scale epitaxial growth and transfer of monolayer MoS has attracted great attention in recent years. Here, we report the wafer-scale epitaxial growth of highly oriented continuous and uniform monolayer MoS films on single-crystalline sapphire wafers by chemical vapor deposition (CVD) method. The epitaxial film is of high quality and stitched by many 0°, 60° domains and 60°-domain boundaries. Moreover, such wafer-scale monolayer MoS films can be transferred and stacked by a simple stamp-transfer process, and the substrate is reusable for subsequent growth. Our progress would facilitate the scalable fabrication of various electronic, valleytronic, and optoelectronic devices for practical applications.
Well-defined Li(4)Ti(5)O(12) nanosheets terminated with rutile-TiO(2) at the edges were synthesized by a facile solution-based method and revealed directly at atomic resolution by an advanced spherical aberration imaging technique. The rutile-TiO(2) terminated Li(4)Ti(5)O(12) nanosheets show much improved rate capability and specific capacity compared with pure Li(4)Ti(5)O(12) nanosheets when used as anode materials for lithium ion batteries. The results here give clear evidence of the utility of rutile-TiO(2) as a carbon-free coating layer to improve the kinetics of Li(4)Ti(5)O(12) toward fast lithium insertion/extraction. The carbon-free nanocoating of rutile-TiO(2) is highly effective in improving the electrochemical properties of Li(4)Ti(5)O(12), promising advanced batteries with high volumetric energy density, high surface stability, and long cycle life compared with the commonly used carbon nanocoating in electrode materials.
Key indicators: single-crystal X-ray study; T = 293 K; mean (P-O) = 0.001 A ˚ ; disorder in solvent or counterion; R factor = 0.032; wR factor = 0.075; data-to-parameter ratio = 36.0. Single crystals of the title compound, trisodium divanadium-(III) tris(orthophosphate), were grown from a self-flux in the system Na 4 P 2 O 7-NaVP 2 O 7. Na 3 V 2 (PO 4) 3 belongs to the family of NASICON-related structures and is built up from isolated [VO 6 ] octahedra (3. symmetry) and [PO 4 ] tetrahedra (.2 symmetry) interlinked via corners to establish the framework anion [V 2 (PO 4) 3 ] 3À. The two independent Na + cations are partially occupied [site-occupancy factors = 0.805 (18) and 0.731 (7)] and are located in channels with two different oxygen environments, viz sixfold coordination for the first (3. symmetry) and eightfold for the second (.2 symmetry) Na + cation. Related literature For structures and properties of complex phosphates with general formula Na 3 M III 2 (PO 4) 3 (M III = Sc, Fe, Cr), see: Collin et al. (1986); Genkina et al. (1991); Lazoryak et al. (1980); Lucazeau et al. (1986); Masquelier et al. (1992); Susman et al. (1983). For preparation of NaVP 2 O 7 which was used as an educt for crystal growth of the title compound, see: Zatovsky et al. (1999). Experimental Crystal data Na 3 V 2 (PO 4) 3 M r = 455.76 Trigonal, R3c a = 8.7288 (2) A ˚ c = 21.8042 (7) A ˚ V = 1438.73 (7) A ˚ 3 Z = 6 Mo K radiation = 2.66 mm À1 T = 293 K 0.20 Â 0.15 Â 0.10 mm Data collection Oxford Diffraction Xcalibur-3 CCD diffractometer Absorption correction: multi-scan (Blessing, 1995) T min = 0.635, T max = 0.780 12580 measured reflections 1331 independent reflections 1153 reflections with I > 2(I) R int = 0.063
Surface dissolution of manganese is a long-standing issue hindering the practical application of spinel LiMn2O4 cathode material, while few studies concerning the crystal structure evolution at the surface area have been reported. Combining X-ray photoelectron spectroscopy, electron energy loss spectroscopy, scanning transmission electron microscopy, and density functional theory calculations, we investigate the chemical and structural evolutions on the surface of a LiMn2O4 electrode upon cycling. We found that an unexpected Mn3O4 phase was present on the surface of LiMn2O4 via the application of an advanced electron microscopy. Since the Mn3O4 phase contains 1/3 soluble Mn2+ ions, formation of this phase contributes significantly to the Mn2+ dissolution in a LiMn2O4 electrode upon cycling. It is further found that the Mn3O4 appears upon charge and disappears upon discharge, coincident with the valence change of Mn. Our results shed light on the importance of stabilizing the surface structure of cathode material, especially at the charged state. The understanding of the manganese dissolution reaction that occurs in the LiMn2O4 can certainly be extended to other oxide cathodes.
Electrochemical energy storage devices with a high energy density are an important technology in modern society, especially for electric vehicles. The most effective approach to improve the energy density of batteries is to search for high-capacity electrode materials. According to the concept of energy quality, a high-voltage battery delivers a highly useful energy, thus providing a new insight to improve energy density. Based on this concept, a novel and successful strategy to increase the energy density and energy quality by increasing the discharge voltage of cathode materials and preserving high capacity is proposed. The proposal is realized in high-capacity Li-rich cathode materials. The average discharge voltage is increased from 3.5 to 3.8 V by increasing the nickel content and applying a simple after-treatment, and the specific energy is improved from 912 to 1033 Wh kg . The current work provides an insightful universal principle for developing, designing, and screening electrode materials for high energy density and energy quality.
Two-dimensional molybdenum disulfide (MoS 2 ) is an emergent semiconductor with great potential in next-generation scaled-up electronics, but the production of high-quality monolayer MoS 2 wafers still remains a challenge. Here, we report an epitaxy route toward 4 in. monolayer MoS 2 wafers with highly oriented and large domains on sapphire. Benefiting from a multisource design for our chemical vapor deposition setup and the optimization of the growth process, we successfully realized material uniformity across the entire 4 in. wafer and greater than 100 μm domain size on average. These monolayers exhibit the best electronic quality ever reported, as evidenced from our spectroscopic and transport characterizations. Our work moves a step closer to practical applications of monolayer MoS 2 .
For LiMO 2 (M ¼ Co, Ni, Mn) cathode materials, lattice parameters, a(b), contract during charge. Here we report such changes in opposite directions for lithium molybdenum trioxide (Li 2 MoO 3 ). A 'unit cell breathing' mechanism is proposed based on crystal and electronic structural changes of transition metal oxides during charge-discharge. Metal-metal bonding is used to explain such 'abnormal' behaviour and a generalized hypothesis is developed. The expansion of the metal-metal bond becomes the controlling factor for a(b) evolution during charge, in contrast to the shrinking metal-oxygen bond as controlling factor in 'normal' materials. The cation mixing caused by migration of molybdenum ions at higher oxidation state provides the benefits of reducing the c expansion range in the early stage of charging and suppressing the structure collapse at high voltage charge. These results may open a new strategy for designing layered cathode materials for high energy density lithium-ion batteries.
Core/shell nanocatalysts are ac lass of promising materials,w hicha chieve the enhanced catalytic activities through the synergy between ligand effect and strain effect. However,i th as been challenging to disentangle the contributions from the two effects,whichhinders the rational design of superior core/shell nanocatalysts.H erein, we report precise synthesis of PdCu/Ir core/shell nanocrystals,w hichc an significantly boost oxygen evolution reaction (OER) via the exclusive strain effect. The heteroepitaxial coating of four Ir atomic layers onto PdCu nanoparticle gives arelatively thickIr shell eliminating the ligand effect, but creates ac ompressive strain of ca. 3.60%. The strained PdCu/Ir catalysts can deliver al ow OER overpotential and ah igh mass activity.D ensity functional theory (DFT) calculations reveal that the compressive strain in Ir shell downshifts the d-band center and weakens the binding of the intermediates,c ausing the enhanced OER activity.The compressive strain also boosts hydrogen evolution reaction (HER) activity and the strained nanocrystals can be served as excellent catalysts for both anode and cathode in overall water-splitting electrocatalysis.
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