8 research outputs found
Self-Limiting Lithiation in Silicon Nanowires
The rates of charging and discharging in lithium-ion batteries (LIBs) are critically controlled by the kinetics of Li insertion and extraction in solid-state electrodes. Silicon is being intensively studied as a high-capacity anode material for LIBs. However, the kinetics of Li reaction and diffusion in Si remain unclear. Here we report a combined experimental and theoretical study of the lithiation kinetics in individual Si nanowires. By using <i>in situ</i> transmission electron microscopy, we measure the rate of growth of a surface layer of amorphous Li<sub><i>x</i></sub>Si in crystalline Si nanowires during the first lithiation. The results show the self-limiting lithiation, which is attributed to the retardation effect of the lithiation-induced stress. Our work provides a direct measurement of the nanoscale growth kinetics in lithiated Si, and has implications on nanostructures for achieving the high capacity and high rate in the development of high performance LIBs
Tough Germanium Nanoparticles under Electrochemical Cycling
Mechanical degradation of the electrode materials during electrochemical cycling remains a serious issue that critically limits the capacity retention and cyclability of rechargeable lithium-ion batteries. Here we report the highly reversible expansion and contraction of germanium nanoparticles under lithiation–delithiation cycling with <i>in situ</i> transmission electron microscopy (TEM). During multiple cycles to the full capacity, the germanium nanoparticles remained robust without any visible cracking despite ∼260% volume changes, in contrast to the size-dependent fracture of silicon nanoparticles upon the first lithiation. The comparative <i>in situ</i> TEM study of fragile silicon nanoparticles suggests that the tough behavior of germanium nanoparticles can be attributed to the weak anisotropy of the lithiation strain at the reaction front. The tough germanium nanoparticles offer substantial potential for the development of durable, high-capacity, and high-rate anodes for advanced lithium-ion batteries
Tough Germanium Nanoparticles under Electrochemical Cycling
Mechanical degradation of the electrode materials during electrochemical cycling remains a serious issue that critically limits the capacity retention and cyclability of rechargeable lithium-ion batteries. Here we report the highly reversible expansion and contraction of germanium nanoparticles under lithiation–delithiation cycling with <i>in situ</i> transmission electron microscopy (TEM). During multiple cycles to the full capacity, the germanium nanoparticles remained robust without any visible cracking despite ∼260% volume changes, in contrast to the size-dependent fracture of silicon nanoparticles upon the first lithiation. The comparative <i>in situ</i> TEM study of fragile silicon nanoparticles suggests that the tough behavior of germanium nanoparticles can be attributed to the weak anisotropy of the lithiation strain at the reaction front. The tough germanium nanoparticles offer substantial potential for the development of durable, high-capacity, and high-rate anodes for advanced lithium-ion batteries
Tough Germanium Nanoparticles under Electrochemical Cycling
Mechanical degradation of the electrode materials during electrochemical cycling remains a serious issue that critically limits the capacity retention and cyclability of rechargeable lithium-ion batteries. Here we report the highly reversible expansion and contraction of germanium nanoparticles under lithiation–delithiation cycling with <i>in situ</i> transmission electron microscopy (TEM). During multiple cycles to the full capacity, the germanium nanoparticles remained robust without any visible cracking despite ∼260% volume changes, in contrast to the size-dependent fracture of silicon nanoparticles upon the first lithiation. The comparative <i>in situ</i> TEM study of fragile silicon nanoparticles suggests that the tough behavior of germanium nanoparticles can be attributed to the weak anisotropy of the lithiation strain at the reaction front. The tough germanium nanoparticles offer substantial potential for the development of durable, high-capacity, and high-rate anodes for advanced lithium-ion batteries
Tough Germanium Nanoparticles under Electrochemical Cycling
Mechanical degradation of the electrode materials during electrochemical cycling remains a serious issue that critically limits the capacity retention and cyclability of rechargeable lithium-ion batteries. Here we report the highly reversible expansion and contraction of germanium nanoparticles under lithiation–delithiation cycling with <i>in situ</i> transmission electron microscopy (TEM). During multiple cycles to the full capacity, the germanium nanoparticles remained robust without any visible cracking despite ∼260% volume changes, in contrast to the size-dependent fracture of silicon nanoparticles upon the first lithiation. The comparative <i>in situ</i> TEM study of fragile silicon nanoparticles suggests that the tough behavior of germanium nanoparticles can be attributed to the weak anisotropy of the lithiation strain at the reaction front. The tough germanium nanoparticles offer substantial potential for the development of durable, high-capacity, and high-rate anodes for advanced lithium-ion batteries
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Supplementary Material
In Situ Transmission Electron Microscopy Study of Electrochemical Sodiation and Potassiation of Carbon Nanofibers
Carbonaceous materials have great
potential for applications as
anodes of alkali-metal ion batteries, such as Na-ion batteries and
K-ion batteries (NIB and KIBs). We conduct an in situ study of the
electrochemically driven sodiation and potassiation of individual
carbon nanofibers (CNFs) by transmission electron microscopy (TEM).
The CNFs are hollow and consist of a bilayer wall with an outer layer
of disordered-carbon (<i>d</i>-C) enclosing an inner layer
of crystalline-carbon (<i>c</i>-C). The <i>d</i>-C exhibits about three times volume expansion of the <i>c</i>-C after full sodiation or potassiation, thus suggesting a much higher
storage capacity of Na or K ions in <i>d</i>-C than <i>c</i>-C. For the bilayer CNF-based electrode, a steady sodium
capacity of 245 mAh/g is measured with a Coulombic efficiency approaching
98% after a few initial cycles. The in situ TEM experiments also reveal
the mechanical degradation of CNFs through formation of longitudinal
cracks near the <i>c</i>-C/<i>d</i>-C interface
during sodiation and potassiation. Geometrical changes of the tube
are explained by a chemomechanical model using the anisotropic sodiation/potassiation
strains in <i>c</i>-C and <i>d</i>-C. Our results
provide mechanistic insights into the electrochemical reaction, microstructure
evolution and mechanical degradation of carbon-based anodes during
sodiation and potassiation, shedding light onto the development of
carbon-based electrodes for NIBs and KIBs
Two-Phase Electrochemical Lithiation in Amorphous Silicon
Lithium-ion batteries have revolutionized portable electronics
and will be a key to electrifying transport vehicles and delivering
renewable electricity. Amorphous silicon (<i>a</i>-Si) is
being intensively studied as a high-capacity anode material for next-generation
lithium-ion batteries. Its lithiation has been widely thought to occur
through a single-phase mechanism with gentle Li profiles, thus offering
a significant potential for mitigating pulverization and capacity
fade. Here, we discover a surprising two-phase process of electrochemical
lithiation in <i>a</i>-Si by using <i>in situ</i> transmission electron microscopy. The lithiation occurs by the movement
of a sharp phase boundary between the <i>a</i>-Si reactant
and an amorphous Li<sub><i>x</i></sub>Si (<i>a</i>-Li<sub><i>x</i></sub>Si, <i>x</i> ∼ 2.5)
product. Such a striking amorphous–amorphous interface exists
until the remaining <i>a</i>-Si is consumed. Then a second
step of lithiation sets in without a visible interface, resulting
in the final product of <i>a</i>-Li<sub><i>x</i></sub>Si (<i>x</i> ∼ 3.75). We show that the two-phase
lithiation can be the fundamental mechanism underpinning the anomalous
morphological change of microfabricated <i>a</i>-Si electrodes,
i.e., from a disk shape to a dome shape. Our results represent a significant
step toward the understanding of the electrochemically driven reaction
and degradation in amorphous materials, which is critical to the development
of microstructurally stable electrodes for high-performance lithium-ion
batteries