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The document discusses the development of a silicon oxide-carbon (SiOx/C) nanocomposite for use as a stable anode material in lithium-ion batteries (LIBs). The authors detail a method for controllable oxidation of silicon particles with fresh surfaces through hydrothermal treatment, resulting in improved electrochemical performance and cycling stability. The SiOx/C composite demonstrated a high reversible capacity and maintained significant capacity retention after multiple cycles, indicating its potential for commercial applications in next-generation LIBs.

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The document discusses the development of a silicon oxide-carbon (SiOx/C) nanocomposite for use as a stable anode material in lithium-ion batteries (LIBs). The authors detail a method for controllable oxidation of silicon particles with fresh surfaces through hydrothermal treatment, resulting in improved electrochemical performance and cycling stability. The SiOx/C composite demonstrated a high reversible capacity and maintained significant capacity retention after multiple cycles, indicating its potential for commercial applications in next-generation LIBs.

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pubs.acs.

org/NanoLett Letter

Manipulating Oxidation of Silicon with Fresh Surface Enabling


Stable Battery Anode
Gaofeng Ge,∥ Guocheng Li,∥ Xiancheng Wang, Xiaoxue Chen, Lin Fu, Xiaoxiao Liu, Eryang Mao,
Jing Liu, Xuelin Yang, Chenxi Qian, and Yongming Sun*
Cite This: Nano Lett. 2021, 21, 3127−3133 Read Online

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ABSTRACT: Silicon (Si)-based material is a promising anode


material for next-generation lithium-ion batteries (LIBs). Herein,
we report the fabrication of a silicon oxide−carbon (SiOx/C)
nanocomposite through the reaction between silicon particles with
fresh surface and H2O in a mild hydrothermal condition, as well as
conducting carbon coating synchronously. We found that control-
lable oxidation could be realized for Si particles to produce
uniform SiOx after the removal of the native passivation layer. The
uniform oxidation and conductive coating offered the as-fabricated
SiOx/C composite good stability at both particle and electrode
level over electrochemical cycling. The as-fabricated SiOx/C
composite delivered a high reversible capacity of 1133 mAh g−1
at 0.5 A g−1 with 89.1% capacity retention after 200 cycles. With 15
wt % SiOx/C composite, graphite-SiOx/C hybrid electrode displayed a high reversible specific capacity of 496 mAh g−1 and stable
electrochemical cycling with a capacity retention of 90.1% for 100 cycles.
KEYWORDS: lithium-ion batteries, silicon-based anode, controllable oxidation, capacity, cycling stability

L ithium-ion batteries (LIBs) have been widely used as


dominating power sources in portable electronics and are
penetrating into the electrochemical vehicles and grid energy
surface area, leading to continuous consumption of active Li
and electrolyte, growth of thick SEI, and an increase of
electrode impedance (Figure S1a).18−20
storage.1−4 The ever-increasing energy demand requires higher Effectively addressing the inherent problems of Si NPs, Si/C
energy density of LIBs, which requires the development of new nanocomposites have triggered extensive scientific re-
electrode materials with higher capacity.5−9 In the past years, search.21−25 They can not only improve the electrical
research has been widely conducted on Si-based materials to conductivity but also alleviate the volume change upon cycling
replace the traditional graphite anode materials due to their processes, exhibiting improved electrochemical perform-
much higher theoretical capacity (4200 mAh g−1 for Si versus ance.26,27 On the other hand, silicon suboxides (SiOx) show
372 mAh g−1 for graphite), low cost, and abundance in outstanding virtue of less volume expansion/shrinkage in
resources.10−13 Unfortunately, the commercial application of comparison to Si and can suppress the undesirable side
Si-based materials is hindered by several severe issues, reactions and improve the electrochemical cycling stabil-
including low electrical conductivity, dramatic volume change ity.28−30 The oxygen in SiOx can react with Li+ generating
(>300%), and unstable solid electrolyte interphase (SEI).14−16 inactive Li2O and lithium silicates during the initial lithiation
Intrinsically, large volume expansion and contraction during process, which are beneficial for buffering volume expansion
the lithiation/delithiation processes cause the fracture and and maintaining structural stability of the active material
pulverization of Si at both the particle and electrode levels, and during cycling.28,30 Meanwhile, the SEI layer formed on the
thus the inferior cycling stability.7,17 Meanwhile, fresh surface surface of the SiOx anode is more stable and intact than that on
of Si is exposed accompanied by the fracture of the originally pure Si (Figure S1b). Therefore, although the specific capacity
formed SEI, where new SEI reforms in the following charge/
discharge cycles. Such a process consumes active lithium and Received: January 26, 2021
electrolyte continuously and the as-formed thick SEI weakens Revised: March 15, 2021
the lithium-ion diffusion, which further results in degradation Published: March 18, 2021
of electrochemical performance.18 Although Si nanoparticles
(Si NPs) can effectively avoid the particle fracture,7 the
problem of serious side reactions still exists due to its high

© 2021 American Chemical Society https://doi.org/10.1021/acs.nanolett.1c00317


3127 Nano Lett. 2021, 21, 3127−3133
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of SiOx is somehow reduced in comparison to pure Si, the the oxidation process and degree can be easily regulated.
cycling stability is remarkably enhanced. With the combined Besides, synchronous carbon coating was realized by
advantage of composite of SiOx and carbon, SiOx/C introducing carbon sources into the solution for hydrothermal
nanocomposites have been shown their advantage in realizing treatment and the SiOx/C composite was fabricated after
stable electrode with reasonably high capacity, exhibiting good further annealing (Figure 1b).
commercial application prospect (Figure S1c).31,32 However, After the removal of the native passivation layer on the Si
to date there lacks a facile and mild approach to regulate the particle, one can easily regulate the oxidation of Si. On the
oxygen content in SiOx during the material’s fabrication. A low basis of the framework of Cabrera−Mott mechanism, the
content of oxygen cannot guarantee the effective suppression controllable oxidation process under a hydrothermal condition
of volume change while a high content of oxygen would result is illustrated (Figure 1c).33 Numerous highly reactive water
in severe capacity reduction and large voltage hysteresis in and oxygen molecules surround the surface of uncontaminated
voltage curves.28 Si. Polar water molecules preferentially adhere to the surface
Herein, we reveal the important role of fresh surface in silanol groups, inducing the break of neighboring SiSi bond
regulating the oxidation of Si and realizing controllable adjacent to SiOH bond due to its strong polarity while
oxidation and in situ carbon coating to form SiOx/C without any damage to the hydrophobic SiH surface bonds
composites though a facile one-step hydrothermal process (step 2). Then an electron from the broken chemical bond
and subsequent carbonization using Si waste from solar transfers to the adhesive O2 and makes it electronegative (step
photovoltaic industry as the raw material. The prepared 3). Driven by the generated electrostatic potential, the
material featured a uniform composite of SiOx and carbon. The resultant O2− migrates toward the broken SiSi bond (step
uniform oxidation and in situ carbon coating are beneficial for 4), which causes the oxidation of this chemical bond and an
improving the electrochemical performance of Si-based anodes adjacent SiSi bond (step 5).33 Here, the etching of pristine
for LIBs. As expected, the as-obtained SiOx/C composite passivation layer of bare Si overturns the feasibility of the
anode not only delivers high specific capacity but also above-mentioned surface chemical evolution and favors for in
manifests excellent cycling stability, thus providing a feasible situ fabrication of C coating layer. In addition, elevated
approach for fabricating high-performance anodes for the pressure and high humidity provided by hydrothermal
forthcoming generation LIBs. treatment further exacerbate the kinetics and thermodynamics


of oxidation behavior.
Si waste from the photovoltaic industry was used as the Si
RESULTS AND DISCUSSION
resource for the fabrication of SiOx/C composite. The Si
There exists a dense layer of SiOx on the bare Si surface powder before (namely initial Si) and after (namely pristine
(Figure 1a). This dense passivation layer insulates the active Si) the removal of the passivation layer showed similar
silicon from oxygen in the environment and inhibits further morphology of irregular particles with size range between 100
oxidation. Thus, bare Si particles cannot be oxidized under to 300 nm observed from scanning electron microscopy (SEM,
hydrothermal condition (Figure S2a, b). After the removal of Figure S3a,b). The SiOx/C composite was successfully
the passivation layer, Si particles with a fresh surface is easily fabricated after the hydrothermal treatment of Si particles
oxidized into SiOx under a mild hydrothermal condition and with fresh surface and the following thermal annealing in Ar
atmosphere. X-ray diffraction (XRD) pattern of the SiOx/C
composite demonstrate typical characteristic peaks at 28.4,
47.3, 56.1, 69.1, 76.4, and 88.0° for crystalline Si (PDF #99-
0092) and a broad bump at ∼23° arising from the silicon oxide
(Figure 2a).21,34 In contrast, only crystalline Si phase was
observed for the pristine Si. A broad XRD peak indicative for
silicon oxidation was shown for Si particles with fresh surface
after the same treatment as the SiOx/C composite except for C
coating (Figure S4a). This result indicates an ineligible amount
of oxidation of Si with fresh surface during the hydrothermal
treatment. With the increase of oxidation degree of silicon, the
peak for silicon oxidation was obviously enhanced, accom-
panied by reduced intensity of the characteristic peaks for
crystalline Si (Figure S4b). According to the electron probe
microanalysis (EPMA), oxygen content in initial Si and SiOx/
C composite was 5.7 wt % and 22.7 wt %, respectively.
Calculated based on the result of thermogravimetric analysis
(TGA), the carbon content in the SiOx/C composite was 15
wt % (Figure S5). X-ray photoelectron spectroscopy (XPS)
was conducted to verify the chemical state evolution of Si from
the pristine Si to the SiOx/C composite. Signals for Si, O, and
C elements are observed for the SiOx/C composite (Figure
Figure 1. (a) Dense passivation layer on the Si surface, which S6a), suggesting the elemental components of the product.
prevents its further oxidation. (b) Schematic illustration of control- The strong carbon signal indicates the successful surface
lable oxidation of Si with fresh surface and synchronous carbon carbon coating on Si particles (Figure S6b). The Si signal is
coating. (c) Schematic of the controllable oxidation under hydro- relatively weak since XPS detects the information on materials
thermal condition for Si particles with a fresh surface. surface and SiOx is protected by the surficial carbon layer/
3128 https://doi.org/10.1021/acs.nanolett.1c00317
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Figure 2. (a) XRD patterns of the starting Si material and the SiOx/C composite. (b) High-resolution Si 2p XPS spectra of the pristine Si and the
SiOx/C composite. (c) SEM image of the SiOx/C composite. (d) High-magnification TEM and (e) HRTEM image of the SiOx/C composite
(enlarged view of the circled area in panel d). (f) HAADF-STEM image of a SiOx/C composite particle, and (g−j) the corresponding EDS
elemental mapping images of Si, O, and C elements.

Figure 3. Electrochemical performance of the SiOx/C composite. (a) Capacity-cycle number plots of the SiOx/C composite and pristine Si at 0.5 A
g−1. The current density for the initial two activation cycles is 0.05 A g−1. (b) Voltage profiles of the SiOx/C electrode at different cycles. (c) Rate
capabilities of the SiOx/C and pristine Si electrodes at various current densities from 0.5 to 2.5 A g−1. (d) CV curves of the SiOx/C electrode at
different scan rates from 0.01 to 0.04 mV s−1. (e) Determination of b-value through the fitted linear model of log i and log v on redox peaks of the
SiOx/C electrode. (f) Cycling performance of the graphite−SiOx/C hybrid and pure graphite electrodes with the same areal capacity fixed at 1 mAh
cm−2. The electrodes were cycled at 0.02 A g−1 for the initial two activation cycles and at 0.08 A g−1 for the subsequent cycles. (g) Galvanostatic
voltage profiles of the graphite−SiOx/C electrode at different cycles.

embedded in the carbon matrix. In contrast, the pristine Si resolution Si 2p XPS spectrum for the SiOx/C composite
powder shows a very weak signal for C and the O signal comes (Figure 2b), a broad peak in the binding energy range of 101−
from the surficial oxidation of the pure Si sample. In the high- 107 eV is fitted to Si+, Si2+, Si3+ and Si4+, showing various
3129 https://doi.org/10.1021/acs.nanolett.1c00317
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oxidation states of the amorphous SiOx. The intensity for Si0 and cycling stability. Once the Si was overoxidized, the
peak in the range of 97−101 eV is negligible, suggesting the capacity dropped drastically (Figure S12). The uniform
considerable oxidation of Si in the SiOx/C composite. In oxidation of Si is beneficial for buffering the volume change
contrast, the bare Si shows obvious peaks for both SiOx and Si, during the repeated alloy/dealloy reactions and improving the
suggesting the slight oxidation of Si during its rest in the stability of active materials. Also, the carbon framework not
ambient condition. The significantly enhanced intensity of only provides good electronic conductivity but also suppresses
peak related to SiOx and weakened intensity of peak to Si−Si the side reactions between the active materials and electrolyte.
bond in the SiOx/C sample indicate that crystalline Si suffers Therefore, the electrochemical stability of the SiOx/C
oxidation during the fabrication. The morphology and composite is much enhanced. The galvanostatic voltage
structure information on the SiOx/C composite have been profiles of the SiOx/C composite electrode demonstrated
investigated by scanning electron microscope (SEM) and characteristic voltage plateaus of Si-based materials (Figures 3b
transmission electron microscope (TEM) coupled with energy and S13). The voltage profiles overlapped well for the initial 20
dispersive X-ray (EDX) elemental mapping. The SiOx/C cycles for the SiOx/C composite electrode. These character-
composite image shows densely packed secondary particles istic voltage profiles remained for 500 cycles with only slightly
with amorphous carbon coating (Figure S7) in the size of increased voltage polarization due to the decay of the counter
several micrometers (Figures 2c and S7), which is quite Li metal electrode in the SiOx/C||Li half cell. This result
different from that of the pristine Si particles with loose illustrated prominent cycling stability of the SiOx/C electrode.
agglomeration (Figure S3b). Transmission electron micro- In contrast, large voltage polarization was observed for the
scope (TEM) investigation was further conducted to pristine Si electrode after only five cycles (Figure S14). The
investigate the structure and component of the SiOx/C superiority in electrochemical performance of the as-fabricated
composite and pristine Si (Figures S9 and S10). The dark SiOx/C composite to pristine Si was also verified by their
area and gray area corresponded to SiOx nanoparticles and the distinct rate capability (Figure 3c). Except for the first four
carbon in the TEM image, respectively (Figure 2d and S9). cycles, the SiOx/C electrode delivered a higher specific
The results show that the SiOx nanoparticles were uniformly capacity than the pristine Si electrode under almost all of the
embedded in a carbon matrix in the composite secondary tested current density conditions. For example, the reversible
particle. In the high-resolution TEM image, the crystalline specific capacity was 970 mAh g−1 for the SiOx/C electrode at
region with 3.1 Å spacing lattice fringe was observed, which 2.5 A g−1, which was significantly higher than 498 mAh g−1 for
ascribed to the (111) plane for Si. These crystalline regions pristine Si electrode (Figure 3c). The voltage profiles of two
were surrounded by amorphous regions (Figure 2e), again samples at different current density were also compared,
revealing the partial oxidation of Si in the SiOx/C composite. further verifying the advance of the SiOx/C composite in rate
To further investigate the microstructure of the SiOx/C capacity (Figure S15a,b). Higher overpotential and faster
composite, the high-angle annular dark-field scanning trans- capacity decay for the pristine Si can be attributed to the
mission electron microscopy (HAADF-STEM) and element sluggish kinetics of alloy/dealloy reactions. For the SiOx/C
mapping were performed. As shown in Figure 2f−j, several composite, the carbon matrix enhanced the conductivity of the
SiOx particles were embedded in a carbon matrix in a SiOx/C entire material and enabled fast reaction kinetics.
composite particle. Si and O elements were evenly distributed To further investigate the structural advantage of the SiOx/C
throughout the core of the SiOx/C composite particle, composite in reaction kinetics during the electrochemical
indicating uniform oxidation of Si. A line scanning test for measurement, cyclic voltammetry (CV) investigation was
Si, O, and C elements was further conducted (Figure S11). conducted for the SiOx/C composite and the pristine Si
The results indicated that the signal of C went across the entire electrodes in the voltage range of 0.01−1 V with different scan
scan line, confirming the intact carbon coating layer on SiOx rates from 0.01 to 0.04 mV s−1. The CV profiles were recorded
particles, which provided good conductivity and worked the and analyzed as shown in Figure 3d and Figure S16a. At all
volume change buffer structure for the SiOx/C nanocomposite. measured rates for the SiOx/C composite, there existed a main
The electrochemical performance of the as-fabricated SiOx/ cathodic peak at ∼0.2 V and two main anodic peaks at ∼0.4
C composite was investigated by galvanostatic charge/ and ∼0.5 V, respectively, corresponding to the alloying and
discharge measurement. All mentioned capacities are based dealloying processes of the LixSi phases (Figure 3d). For the
on the mass of the SiOx/C composite in the electrode. Figure pristine Si electrode, an additional peak at ∼0.1 V was
3a shows the capacity-cycle number plots for the SiOx/C recorded, which might be ascribed to the insertion of Li+ into
composite and pristine Si electrodes cycled at 0.5 A g−1. polycrystalline silicon (Figure S16a).35,36 According to
Although the partial oxidation of Si to SiOx and the previous research, the correlation between scan rates (v) and
introduction of carbon decrease the capacity to a certain peak current (i) can be expressed by a power-law function37,38
extent, the cycling stability of the SiOx/C composite is
significantly enhanced in comparison to the pristine Si. A i = avb
reversible specific capacity of 1133 mAh g−1 was achieved for log i = b log v + log a
the SiOx/C electrode at 0.5 A g−1 after the initial two
activation cycles at 0.05 A g−1. After 500 cycles, the reversible where a and b represent variable parameters. Generally, the b-
capacity of the SiOx/C composite was still at 917 mAh g−1, value of 0.5 indicates a diffusion-controlled interfacial reaction
with a capacity retention of 80.9% and a capacity decay rate of behavior while a b-value of 1 implies a nondiffusion controlled
0.038%. In contrast, although the pristine Si electrode displays capacitive process.39,40 On the basis of the fitted linear model
a high initial capacity of 1699 mAh g−1, it lost nearly all its of log i and log v in which the slopes represented b-values, the
capacity after 500 cycles, showing a very low capacity retention slopes of reduction and oxidation peaks were fitted to 1.0884
of 23.5%. Here, the Si was appropriately oxidized in the SiOx/ and 1.09641 for the SiOx/C composite (Figure 3e), illustrating
C composite, achieving a dynamic balance between capacity the kinetics dominated by a capacitive process. The analogous
3130 https://doi.org/10.1021/acs.nanolett.1c00317
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Figure 4. Cross-sectional and top-view SEM images of the pristine Si electrode (a,c) before and (b,d) after 50 cycles at 0.5 A g−1. Cross-sectional
and top-view SEM images of the SiOx/C electrode (e,g) before and (f,h) after 50 cycles at 0.5 A g−1 (scale bar, 10 μm). (i) HAADF-STEM and (j−
l) corresponding EDS elemental mapping images of the SiOx/C electrode after 100 cycles at 0.5 A g−1.

values for the pristine Si electrode were 0.61738 and 0.51119 pure graphite. The graphite-SiOx/C hybrid delivered a high
(Figure S16b), respectively, indicating that the kinetics were reversible specific capacity of 496 mAh g−1, 50% higher than
primarily diffusion-controlled interfacial reaction behaviors. that of the tested graphite. Meanwhile, graphite-SiOx/C hybrid
These results intrinsically validate the enhanced reaction displayed stable cycling with capacity retention of 90.1% after
kinetics of the SiOx/C composite in comparison to the pristine 100 cycles with fixed areal capacity loading of 1 mAh cm−2.
Si. Observed from the voltage-capacity plots, voltage curves of the
Electrochemical impedance spectroscopy (EIS) was further graphite-SiOx/C hybrid for different cycles overlapped well,
conducted to verify the good electrochemical stability of the and the trend was in good agreement with that of pure
SiOx/C composite. In the Nyquist plots shown in Figure S17, graphite, suggesting good stability during cycling (Figures 3g
the irregular semicircle at high-medium frequency range and S18). The result above indicates the important role of the
represented the interface resistance of SEI and the charge SiOx/C composite in improving the state-of-art LIBs and sheds
transfer resistance at the electrode surface, and the oblique light on its potential application in the next-generation high-
straight line at the low frequency range indicated the ion energy-density LIBs.
conductivity of the electrode. After the initial active cycles, the To verify the good stability of the SiOx/C composite, the
value of the interface resistance of the SiOx/C composite was SiOx/C composite and pristine Si electrodes with similar mass
∼100 Ω, which was significantly smaller than that of the loading (0.9 mg cm−2) after cycling were investigated. As
pristine Si (Figure S17a). After 50 cycles, the interface shown by the cross-sectional SEM images, the thickness of the
resistance of the SiOx/C composite remained stable, indicating pristine Si electrode dramatically increased from 16.5 to 30.5
its good interface stability and stable SEI structure. The μm after 50 cycles (Figure 4a, b). Moreover, the top-view SEM
oxidation of Si relieves the volume change during the images showed rough surface for the pristine Si electrode due
lithiation/delithiation processes, and the in situ formed carbon to the coverage of a thick SEI, and severe cracks were observed
matrix enhanced the conductivity and isolated the direct (Figure 4c,d). These results indicated the rapid mechanical
contact between Si and electrolyte, thus resulting in a stable degradation of electrodes during cycling due to the repeated
SEI. In contrast, the pristine Si anode showed quick increase in large volume expansion and shrinkage, and continuous side
interface resistance, indicating the overincreasing thickness of reactions during cycling. In sharp contrast, the SiOx/C
the SEI due to the continuous side reactions between the electrode displayed a slight increase in thickness from 16.4
electrolyte and materials upon cycling (Figure S17b). to 20.4 μm after 50 cycles (Figure 4e,f) and its surface
Correspondingly, the charge transfer resistance of the SiOx/ remained smooth without very thick SEI and large cracks
C electrode was evidently lower than that of the pristine Si (Figure 4g,h). This result indicated the excellent stability of the
electrode due to the introduction of in situ formed carbon SiOx/C composite electrode during cycling benefited from the
matrix, which could provide abundant charge transfer channels. advantage of low volume change ratio of SiOx in comparison to
To show the practical application of the SiOx/C composite for pristine Si and buffering effect of the carbon matrix. The
the next-generation LIBs, graphite-SiOx/C hybrid electrodes investigation on the morphology and structure of the SiOx/C
were fabricated. The battery cycling was performed at a current composite after cycling was further conducted by high-angle
density of 0.02 A g−1 for the first two cycles and 0.08 A g−1 for annular dark-field scanning transmission electron microscope
the subsequent cycles in Li metal half-cell configuration (HADDF-STEM) and elemental mapping images. Even after
(Figure 3f). Owing to the high specific capacity of SiOx/C 100 cycles at 0.5 A g−1, the initial structure of SiOx in the
composite, the graphite-SiOx/C hybrid with 15 wt % SiOx/C carbon matrix was well preserved without collapsion or rupture
composite showed significantly increased capacity than the (Figure 4i−l). It was observed that the elemental signal for Si
3131 https://doi.org/10.1021/acs.nanolett.1c00317
Nano Lett. 2021, 21, 3127−3133
Nano Letters pubs.acs.org/NanoLett Letter

signal and C overlapped well in a composite particle and the Lin Fu − Wuhan National Laboratory for Optoelectronics,
composite particle maintained its structure without facture, Huazhong University of Science and Technology, Wuhan
suggesting that the active SiOx was well protected by the 430074, China; orcid.org/0000-0001-6834-2881
carbon matrix and the volume change was effectively Xiaoxiao Liu − Wuhan National Laboratory for
suppressed during the long-term cycling. Because of the Optoelectronics, Huazhong University of Science and
regulated oxidation of Si, lithium silicates irreversibly form Technology, Wuhan 430074, China
during the initial lithiation process of SiOx, which functions as Eryang Mao − Wuhan National Laboratory for
a lithium-ion conductive flexible matrix. Moreover, the carbon Optoelectronics, Huazhong University of Science and
matrix also can provide physical confinement for the active Technology, Wuhan 430074, China
material, and alleviate the direction contact between electrolyte Jing Liu − Wuhan National Laboratory for Optoelectronics,
and active material, thus stabilizing the SEI layer and Huazhong University of Science and Technology, Wuhan
eventually improve the overall electrochemical performance 430074, China
of Si electrode. Xuelin Yang − College of Electrical Engineering and New


Energy, China Three Gorges University, Yichang, Hubei
CONCLUSION 443002, China; orcid.org/0000-0001-5626-701X
We explored a facile approach to regulate the oxidation of Si Chenxi Qian − Division of Chemistry and Chemical
particles in a mild condition. Experimentally, we fabricated a Engineering, California Institute of Technology, Pasadena,
SiOx/C composite with controlled oxidation degree using Si California 91125, United States
particles with fresh surface under a mild hydrothermal Complete contact information is available at:
condition followed by thermal annealing. The as-fabricated https://pubs.acs.org/10.1021/acs.nanolett.1c00317
SiOx/C composite featured active SiOx particles embedded in
a carbon matrix, which enhanced the reaction kinetics and Author Contributions

greatly relieved volume variation at both the particle and G.G. and G.L. contributed equally to this work.
electrode level. As expected, the SiOx/C composite maintained Notes
good structural integrity and electrochemical stability for over The authors declare no competing financial interest.


100 charge/discharge cycles. When mixed with graphite, a
graphite-SiOx/C hybrid electrode with 15 wt % SiOx/C ACKNOWLEDGMENTS
displayed a much higher capacity of 496 mAh g−1 than the
This work was supported by National Key R&D Program of
pure graphite and a high capacity retention of 90.1% for 100
China (2018YFB0905400), Major Technological Innovation
cycles. Therefore, the SiOx/C composite exhibits an indelible
Project of Hubei Science and Technology Department
important promotion for the commercial application of high-
(2019AAA164). Y.S. acknowledges the financial support by
capacity Si-based anode for the next generation of high-energy
the Innovation Fund of Wuhan National Laboratory for
lithium-ion batteries.


Optoelectronics of Huazhong University of Science and
Technology. C.Q. acknowledges the support of the Natural
ASSOCIATED CONTENT Sciences and Engineering Research Council of Canada
*
sı Supporting Information (NSERC Postdoctoral Fellowship). The authors would like
The Supporting Information is available free of charge at to thank the Analytical and Testing Center of Huazhong
https://pubs.acs.org/doi/10.1021/acs.nanolett.1c00317. University of Science and Technology (HUST) as well as the
Center for Nanoscale Characterization and Devices of Wuhan
Experimental details and additional characterizations National Laboratory for Optoelectronics (WNLO) for
(PDF) providing the facilities to conduct the characterizations.

■ AUTHOR INFORMATION
Corresponding Author
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