Supercritical CO2 (SCCO2), characterized by gas‐like diffusivity, low surface tension, and excellent mass transfer properties, is applied to create a SiOx/carbon multi‐layer coating on Si particles. Interaction of SCCO2 with Si produces a continuous SiOx layer, which can buffer Si volume change during lithiation/delithiation. In addition, a conformal carbon film is deposited around the Si@SiOx core. Compared to the carbon film produced via a conventional wet‐chemical method, the SCCO2‐deposited carbon has significantly fewer oxygen‐containing functional groups and thus higher electronic conductivity. Three types of carbon precursors, namely, glucose, sucrose, and citric acid, in the SCCO2 syntheses are compared. An eco‐friendly, cost‐effective, and scalable SCCO2 process is thus developed for the single‐step production of a unique Si@SiOx@C anode for Li‐ion batteries. The sample prepared using the glucose precursor shows the highest tap density, the lowest charge transfer resistance, and the best Li+ transport kinetics among the electrodes, resulting in a high specific capacity of 918 mAh g−1 at 5 A g−1. After 300 charge–discharge cycles, the electrode retains its integrity and the accumulation of the solid electrolyte interphase is low. The great potential of the proposed SCCO2 synthesis and composite anode for Li‐ion battery applications is demonstrated.
Encapsulating silicon (Si) nanoparticles with graphene nanosheets in a microspherical structure is proposed to increase electrical conductivity and solve stability issues when using Si as an anode material in lithium-ion batteries (LIBs).
a b s t r a c tSpherical and rod like nanocrystalline Nd 2 O 3 phosphors have been prepared by solution combustion and hydrothermal methods respectively. The Powder X-ray diffraction (PXRD) results confirm that hexagonal A-type Nd 2 O 3 has been obtained with calcination at 900 • C for 3 h and the lattice parameters have been evaluated by Rietveld refinement. Surface morphology of Nd 2 O 3 phosphors show the formation of nanorods in hydrothermal synthesis whereas spherical particles in combustion method. TEM results also confirm the same. Raman studies show major peaks, which are assigned, to F g and combination of A g + E g modes. The PL spectrum shows a series of emission bands at ∼326-373 nm (UV), 421-485 nm (blue), 529-542 nm (green) and 622 nm (red). The UV, blue, green and red emission in the PL spectrum indicates that Nd 2 O 3 nanocrystals are promising for high performance materials and white light emitting diodes (LEDs).
Electrolyte
is a key component in high-voltage lithium-ion batteries
(LIBs). Bis(trifluoromethanesulfonyl)imide-based ionic liquid (IL)/organic
carbonate hybrid electrolytes have been a research focus owing to
their excellent balance of safety and ionic conductivity. Nevertheless,
corrosion of Al current collectors at high potentials usually happens
for this kind of electrolyte. In this study, this long-standing problem
is solved via the modulation of the IL/carbonate ratio and LiPF6 concentration in the hybrid electrolyte. The proposed electrolyte
suppresses Al dissolution and electrolyte oxidation at 5 V (vs Li+/Li) and thus allows for ideal lithiation/delithiation performance
of a high-voltage LiNi0.5Mn1.5O4 (LNMO)
cathode even at 55 °C. The underlying mechanism is examined in
this work. Excellent cycling stability (97% capacity retention) for
an LNMO cathode after 300 cycles is achieved. This electrolyte shows
good wettability toward a polyethylene separator and low flammability.
In addition, satisfactory compatibility with both graphite and Si-based
anodes is confirmed. The proposed electrolyte design strategies have
great potential for applications in high-voltage LIBs.
The use of Si and nitrogen-doped graphene to fabricate composite anodes in lithium-ion batteries (LIBs) is attracting intense attention. However, the reported strategies are limited to achieving a cost-effective, scalable, and facile approach. In particular, many reports on Si/N-graphene (N-Gra) anodes cannot achieve a high first discharge capacity while retaining a high Coulombic efficiency (CE). Herein, we report a Si@N-Gra composite with core−shelled microballs of Si NPs and electrochemically exfoliated graphene by NH 3 as a nitrogen source. We use H 2 and NH 3 to control the O and N content and to optimize the anode performance.
Highly concentrated electrolytes, although promising, are of high cost and show high viscosity and unsatisfactory wettability toward electrodes and separators, making them unfavorable for practical applications. A more rational electrolyte design is thus needed. Here, we investigate moderately concentrated electrolytes and find that the lithium bis(fluorosulfonyl)imide (LiFSI) concentration effects on the capacity, rate capability, and cycling stability of Si anodes in an ethylene carbonate (EC)/diethyl carbonate (DEC) mixed electrolyte are opposite to those in a fluoroethylene carbonate (FEC) electrolyte. The reasons for these results are systematically examined using Raman spectroscopy, transmission electron microscopy, electrochemical impedance spectroscopy, and the galvanostatic intermittent titration technique. A detailed X-ray photoelectron spectroscopy analysis is performed to study the solid electrolyte interphase chemistry. Al corrosion that occurs with the EC/DEC-based electrolyte can be effectively suppressed with the FEC-based electrolyte if an adequate LiFSI concentration is used. In the proposed 2 mLiFSI/FEC electrolyte, the Si anode has reversible capacities of 2630 and 855 mA h g −1 at 0.2 and 5 A g −1 , respectively, and ∼75% capacity retention after 200 cycles (remarkably higher than that obtained with the EC/DEC-based electrolyte). This electrolyte also shows great compatibility with the high-energy-density LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC-811) cathode, allowing a stable charge−discharge of a Si//NMC-811 full cell.
Nanocrystalline Nd(2)O(3):Cu(2+) (2mol %) phosphors have been prepared by a low temperature solution combustion technique. Powder X-ray diffraction (PXRD) results confirm that hexagonal A-type Nd(2)O(3) (900°C, 3h) and the lattice parameters have been evaluated by Rietveld refinement. Surface morphology of as-formed and Cu(2+) doped Nd(2)O(3) phosphors show that the particles are irregular in shape and porous in nature. TEM results also confirm the nature and size of the particles. The EPR spectrum exhibits two resonance signals with effective g values at g(ǀǀ)≈2.12 and g(⊥)≈2.04. The g values indicate that the site symmetry of Cu(2+) ions is octahedral symmetry with elongated tetragonal distortion. Raman studies show major peaks, which are assigned, to F(g) and combination of A(g)+E(g) modes. It is observed that the Raman peaks and intensity have been reduced in Cu(2+) doped samples. UV-Visible absorption spectra exhibit a strong and broad absorption band at ∼240nm. Further, the absorption peak shifts to ∼14nm in Cu(2+) doped samples. The optical band gap is estimated to be 5.28eV for Cu doped Nd(2)O(3) nanoparticles which are higher than the bulk Nd(2)O(3) (4.7eV). This can be attributed to the quantum confinement effect of the nanoparticles.
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