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Carbon 177 (2021) 52e59

Contents lists available at ScienceDirect

Carbon
journal homepage: www.elsevier.com/locate/carbon

A graphene oxide coated sulfide-based solid electrolyte for dendrite-


free lithium metal batteries
Jianwei Li a, Yuanyuan Li a, Jun Cheng b, Qing Sun a, Linna Dai a, Xiangkun Nie a,
Lina Chen b, Guifang Han a, **, Lijie Ci a, b, *
a
Key Laboratory for Liquid-Solid Structural Evolution & Processing of Materials (Ministry of Education), Research Center for Carbon Nanomaterials, School
of Materials Science and Engineering, Shandong University, Jinan, 250061, China
b
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen,
518055, China

a r t i c l e i n f o a b s t r a c t

Article history: Sulfide-based solid electrolyte is one of the most promising solid electrolytes due to its high ionic
Received 29 December 2020 conductivity and wide electrochemical window. However, it suffers from serious interfacial issues with
Received in revised form lithium metal, which hinder the lithium-ion transport during cycling process and increase the interfacial
22 January 2021
resistance and instability. Protection only from Li anode side is not enough since Li enters into the bulk
Accepted 23 January 2021
solid electrolyte resulting reaction and dendrite growth. Herein, we design a graphene oxide (GO) coated
Available online 22 February 2021
solid electrolyte Li7P3S11 particles for stable and efficient all-solid-state battery application. The GO could
partially isolate the Li7P3S11 solid electrolyte from lithium metal. Meanwhile, the GO or rGO reduced by Li
Keywords:
Sulfide-based solid electrolyte
guide the homogeneous growth of Li and increase the cycling stability. Our work provides a facile
Graphene oxide method to fully protect Li7P3S11 in three directions from reaction with Li metal for dendrite-free and
Cycling performance highly stable sulfide-based all-solid-state battery applications. This work might inspire the community
Dendrite-free with new material engineering/design strategies toward practical application in highly stable all solid
state lithium-ion batteries.
© 2021 Elsevier Ltd. All rights reserved.

1. Introduction and superior chemical stability against anode and cathodes. How-
ever, most of oxide-based solid-state electrolytes are still con-
Secondary batteries with improved safety and higher energy fronted with low ionic conductivity and high processing cost
density are in urgent demand in large scale energy storage devices [9e11]. The sulfide-based inorganic solid electrolyte has higher
and electric vehicles applications [1,2]. However, conventional ionic conductivities (103-102 S cm1) due to the high polariz-
batteries employ flammable organic liquid electrolytes suffering ability of sulfide ions, and meanwhile, a wide electrochemically
from severe safety issues such as fire and explosion [3,4]. Recently, stable voltage window [12e20]. Benefiting from its high ionic
all-solid-state batteries (ASSBs) adopting solid-state electrolytes, conductivity, low cost, decent deformability, as well as a facile so-
have been considered as ideal next-generation rechargeable bat- lution synthesizability, the glassy LiePeS sulfide, Li7P3S11 (denoted
teries to fundamentally solve the safety concern and enhance the as LPS) solid electrolyte has received mass attention [21e25].
energy density [5e8]. It has been extensively acknowledged that However, some challenges still need to be overcome for reliable
the electrolyte should meet the following advantages: high ionic ASSBs using the LPS solid electrolyte, mainly including: (1) the LPS
conductivity (>1 mS cm1), wide electrochemical window (>5 V) electrolyte could react with the lithium metal, which increases
interface resistance and results in low Coulomb efficiency [25e27].
(2) lithium dendrites could grow along pores, cracks, grain
boundaries and other defects inside LPS and finally penetrate the
* Corresponding author. Key Laboratory for Liquid-Solid Structural Evolution &
whole electrolyte [28e30]. However, the mechanism for this
Processing of Materials (Ministry of Education), Research Center for Carbon
Nanomaterials, School of Materials Science and Engineering, Shandong University, growth and formation of lithium dendrite in solid electrolyte still
Jinan, 250061, China. remains unclear; (3) Even more, direct growth of lithium dendrites
** Corresponding author. inside the solid electrolyte was observed [30]. The high electrons
E-mail addresses: gfhan@sdu.edu.cn (G. Han), lci@sdu.edu.cn (L. Ci).

https://doi.org/10.1016/j.carbon.2021.01.159
0008-6223/© 2021 Elsevier Ltd. All rights reserved.
J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

conductivity of SSEs might contribute to the formation of Li den- 2.3. Electrochemical measurement
drites, albeit further studies are necessary [31].
To address these issues mentioned above, special attention has Ionic conductivities of Li7P3S11 and x% GO@Li7P3S11 electrolytes
been paid to suppress interface reaction and Li dendrite growth were measured using electrochemical impedance spectroscopy
[32,33]. Yang et al. reported that metal-phosphide-doping (EIS) by a blocking symmetric In/Li7P3S11/In cell. The as-synthesized
restrained the interface reaction between Li and LPS [34]. Howev- powder was cold-pressed under 300 MPa into a pellet with a
er, the preparation process was very complex and not easy to diameter of 10 mm and thickness around 1 mm. Cyclic voltam-
control [35,36]. Graphene or reduced graphene oxide (rGO) were metry (CV) was carried out at a scan rate of 0.1 mV s1 within a
mixed with or coated on Li anode and the layer feature could guide potential range of 0.2e5.0 V. EIS was performed from 100 kHz to
the uniform growth of planar lithium layers instead of random 0.01 Hz. The CV and EIS were carried out using an Autolab analyzer
dendrites [37e39]. These films can also hinder the side reaction (PGSTAT302 N). For all-solid-state batteries assembly, around
between the lithium metal and electrolyte. However, most of these 8e10 mg composite cathode (graphite) were spread and pressed on
reports are based on batteries with liquid electrolyte, and the the one side of the pelletized SE under 300 MPa, after which
protection layer between Li anode and electrolyte could effectively lithium foil was successively attached on the opposite side of SE
suppress the interface reaction. In ASSBs adopting solid-state pellet under 150 MPa. The galvanostatic discharge/charge cycles
electrolytes, Li metal enters into bulk solid electrolyte during were obtained using a battery testing system (Land battery testing
cycling and introduces large amount of Li/electrolyte interface instrument) in the voltage range of 0.1e3 V at the room tempera-
resulting in sever side reaction. Considering the large area of in- ture. LiNbO3-coated LiCoO2 was used as cathode material. The
terfaces between Li metal and bulk solid electrolyte, protection composite of LiNbO3-coated LiCoO2 and LPS with a weight ratio of
only from Li anode side is not enough. A strategy to fully protect 7:3 were uniformly mixed as the working electrode. Metallic Li was
solid electrolyte from reaction with Li and meanwhile inhibit the selected as anode. The assembled ASSLBs were charged and dis-
growth of Li dendrite should be developed. charged in galvanostatic mode at 0.1 C (1 C ¼ 140 mAh g1) in the
Here in this work, a facile method was proposed to form a GO range of 2.8e4.2 V vs Li/Liþ. All processes were carried out in a
coating on top of LPS particle surface then pressed into pellet for glove box.
battery assembly. Due to this GO protection layer, the interfacial
reaction between the LPS electrolyte and lithium metal is miti-
gated. Meanwhile, GO layer could guide or induce the homoge- 3. Results and discussion
neous growth of Li during striping/plating process. Besides, even if
the GO is reduced by Li, it would not mitigate these effects as rGO is The schematic synthesis procedure is shown in Fig. 1(a). GO was
also a good protection material reported. The LieLi symmetrical cell dissolved in ACN to form a solution. Subsequently, Li2S and P2S5
assembled with GO coated LPS electrolyte was stably charged/dis- with a stoichiometric ratio of 7:3 were added and further kept
charged for 300 cycles at the room temperature with a current of stirring at 50  C for 48 h. After evaporation of ACN solution under
0.1 mA cm2. The whole cell demonstrated excellent cycling per- 80  C, the obtained dry powder was heated at 250  C for 1 h. Then
formance with a reversible capacity over 260 mAh g1 and cycling the GO-coated LPS composite electrolyte powder was obtained. It
steadily over 50 cycles. should be noted that the thickness of the GO layer affects the ionic
conductivity of composite powders. Therefore, three different ra-
tios between GO and LPS, i.e. 0.5%, 1% and 2%, were chosen during
2. Experimental synthesis. As can be seen from Fig. 1(b), the control LPS powder is
uniform nanoparticles with size of around 100 nm. When GO is
2.1. Materials synthesis introduced, aggregation of particles are observed with GO wrapped
outside (Fig. 1(cee)). The thickness of GO increased with the
Graphene oxide (GO) was synthesized by a modified Hummers’ increasing of GO content. Most interestingly, the sheet-like struc-
method as we previously reported [40]. Briefly, Li2S and P2S5 with a ture can be clearly observed for the 1% GO@LPS powder, where GO
mole ratio of 7:3 were mixed with GO with different mass ratio (0%, coated on nanoparticles as depicted in Fig. 1(d). This feature dis-
0.5%, 1% and 2%). Then, the mixture was ground thoroughly to get a appears when further increasing the ratio of GO (Fig. 1(e)). These
homogeneous blend. Subsequently, the powder was placed in results confirm that GO is successfully coated/wrapped onto LPS
20 ml acetonitrile solvent under stirring at 50  C for 72 h. After that, particles. High-resolution TEM image (Fig. S1) further demonstrate
the solvent was dried at 80  C for overnight. Then the powder was the ultra-thin GO layers on the top of LPS particle.
further heated at a temperature of 250  C for 1 h and the hybrid To investigate the effect of GO coating on the phase structure of
electrolytes were obtained (marked as x% GO@LPS, and x% is the LPS powders, XRD was conducted and given in Fig. 2(a) and S2.
percentage of GO). All preparation processes were performed in a Main diffraction peaks at 2q ¼ 15.9 , 29.8 , 30.0 , 31.2 , 31.9 and
nitrogen filled glove box. 34.3 can be indexed to Li7P3S11. No significant difference is noticed
after GO coating, which suggests that addition of GO during syn-
thesis does not change the crystal structure of LPS. No peak from GO
2.2. Material characterization (XRD pattern for pure GO is shown in Fig. S3) is found probably due
to its very low amount. Raman was performed to reveal the
Morphologies of coated LPS powder and Li foil after cycling were chemical structure. As exhibited in Fig. 2(b), an obvious peak
characterized by a scanning electron microscope (SEM, JSM-7800F, around 426 cm1 corresponding to PS3 4 unit is observed for the
Hitachi) and a transmission electron microscope (JEOL JEM-2100 F). pristine LPS and GO coated ones, consistent with the XRD results.
The crystalline structure of samples was investigated by X-ray The electrochemical impedance spectroscopy (EIS) of pressed
diffraction using a Miniflex 600 instrument with copper Ka radia- electrolyte pallets are shown in Fig. 2(c). The ionic conductivity (s)
tion and scanning range between 10 and 80 . Raman spectra were of these GO@Li7P3S11 composite solid electrolytes is calculated ac-
conducted on a Renishaw in Via micro-Raman microscope. The X- cording to:
ray photoelectron spectroscopy (XPS, ESCALAB 250) analysis was
performed with Al Ka as the X-ray source. s ¼ L/RS (1)
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J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

Fig. 1. (a) Schematic illustration of the synthesis strategy of GO@LPS composite electrolyte; SEM images of (b) LPS, (c) 0.5% GO@LPS, (d) 1% GO@LPS and (e) 2% GO@LPS solid
electrolytes. (A colour version of this figure can be viewed online.)

Fig. 2. (a) XRD patterns, (b) Raman spectra, (c) Nyquist plots and (d) Time dependence of DC current of LPS and x% GO@LPS composite electrolytes. (A colour version of this figure
can be viewed online.)

where L and S are the thickness and area of the electrolyte pellet, Moreover, it has been reported that the lithium ions can potentially
respectively, and R is the resistance obtained from the EIS mea- find low-energy conducting paths along the interface between the
surement [23]. carbon-based filler and solid state electrolyte [45]. The GO sheet
The calculated ionic conductivities are ~1.01  103 S cm1 for has a number of oxygenated functionalities including epoxy, hy-
LPS, ~1.02  103, 1.11  103 and 0.45  103 S cm1 for 0.5%, 1% droxyl, and carboxyl groups, which are beneficial to Liþ transport.
and 2% GO added LPS, respectively, in which 1% GO@LPS exhibits As the GO content increases (1%), the GO sheets can interconnect to
the highest ionic conductivity. Addition of appropriate amount of form a network, which can facilitate continuous ion conducting
GO slightly enhances the ionic conductivity of LPS. Because various within the composite electrolyte. Table S1 provides a detailed
oxygen functional groups that GO contains can interact with summarization of the ionic conductivity for the Li7P3S11 using the
lithium thiophosphate, it can increase ionic conductivity [41e44]. solution method.

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J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

Electronic conductivities were also measured by the DC method and the cell can be stable up to 600 h of Li plating/stripping without
use blocking electrodes. Fig. 2(d) shows the time dependent DC any significant change (Fig. 3(a)). Magnified details of Fig. 3(a) are
current under a voltage of 1 V. When the blocking electrodes are illustrated in Fig. 3(b) and (c) at the stage of 20e30 h and 90e100 h
adopted, the polarization initially occurs and then the current plating/stripping times, respectively. These figures clearly present
become nearly constant. The calculated electronic conductivity of that the overpotential of the cells from 1% GO@LPS is much lower
the 1% GO@LPS from the constant part is 6.2  108 S cm1. The than that from LPS. Similar short circuit phenomena are found for
ionic conductivity of the electrolyte is about 5 orders of magnitude the cells from LPS with addition of 0.5% and 2% GO but appear at
higher than its electronic conductivity, which suggests that the different times (Fig. S3). Meanwhile, the LPS and 1% GO@LPS was
electronic conductivity could be ignored. systematically tested at a current density of 0.1 mA cm2 with a
To investigate whether this strategy could enhance the perfor- capacity of 1 mAh cm2 (Fig. 3(d)). Li/1% GO@LPS/Li symmetric cell
mance of the electrolyte, Li/x% GO@LPS/Li symmetric batteries exhibits the most stable performance compared to others. The
were assembled and tested at a current density of 0.1 mA/cm2 at critical current density (CCD) is usually adopted to evaluate the
room temperature. As shown in Fig. 3(a), the control cell from LPS dendrite suppression capability of the electrolyte. Fig. S3c shows
exhibits an unstable overpotential of 70 mV, which is quickly the voltageetime curves for the LPS and x% GO@LPS electrolytes.
shorted after 40 h cycles at 0.1 mA cm2. However, for the cell with The critical current densities for the samples with different amount
1% GO@LPS electrolyte, a lower overpotential of 45 mV is observed of GO are shown in Fig. S3c. The CCD of pristine LPS is 0.2 mA cm2.

Fig. 3. (a) Li plating/stripping voltage profiles of Li/Li symmetric batteries with LPS and 1% GO@LPS electrolyte at a current density of 0.1 mA cm 2; (b) and (c) Magnified region in
(a); (d) Typical voltage profiles at 0.1 mA cm2. (e) Cyclic voltammogram of the Li/SE/In cell at a scan rate of 1 mV s1. (A colour version of this figure can be viewed online.)

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J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

With the GO coating, the value increases continuously and reaches contrast, a small change in the total resistance is measurable for cell
the maximum value of 0.6 mA cm2 at 1% GO coating. Therefore the from 1% GO@LPS after 20 h’s (102 U) or even 100 h’s cycle (150 U)
1% GO coating LPS not only increases the ionic conductivity, but also from original sample. It further suggests that x% GO@LPS could
effectively enhances the interfacial stability between electrolyte increase the interface compatibility in the symmetric batteries,
and Li metal, and inhibits the growth of lithium dendrites. In order thus enhance its electrochemical performance.
to figure out whether the addition of GO will affect the electro- As proposed afore and schematically shown in Fig. 5(a), GO
chemical window of LPS, cyclic voltammetry measurement was coated on the surface of LPS particle provides a protection function.
conducted with Li and stainless steel (SS) served as the reference When contacted with Li, GO might be reduced to reduced graphene
and the working electrodes, respectively. The scan rate is 1 mV s1, oxide (rGO) and Li be oxidized to LieO even if the Li dendrite breaks
and the voltage range is from 0.5 to 5 V vs. Li/Liþ. As profiled in the coated rGO layer. The rGO layer ensures the stability at the
Fig. 3(e), the lithium deposition (Li/Liþ) can only be observed at lithium/electrolyte interface and inhibits the growth of lithium
about 0 V and no other peak is observed. It suggests that all samples dendrite, simultaneously. This is confirmed by a clear LieO peak
exhibit a similar electrochemical window up to 5 V and good sta- observed in the XPS result from the LPS electrolyte surface after
bility with lithium. The addition of GO does not affect the voltage cycling, as shown in Fig. S6. Therefore, the advantage of the GO
window of LPS. Therefore, the enhanced performance of 1% coating on the electrolyte is to prevent the Li dendrite growth
GO@LPS electrolyte should be attributed to the GO coating inhib- during the micro-short circuit in the ASSLIBs. To directly get evi-
iting the interfacial side reaction between LPS and lithium anode. dence whether GO/rGO could effectively protect LPS from reaction
To further reveal the evolution of the interface between Li metal with Li metal, XPS analysis was conducted from the Li surface after
and SE during the cycling process, the surface of Li metal surface cycling with LPS and 1% GO@LPS electrolytes for 20 cycles [Fig. 5(b-
before and after the charge-discharge cycles were checked by SEM. f)]. For LPS after cycling, P 2p can be fitted into three different
The original surface of Li metal is very smooth (Fig. 4 (a)). With the species at 126.05, 132.40 and 134.30 eV, which belong to Li3P, P2S4 7
increasing number of cycles, the morphology of Li anode contacting and PS34 , respectively (Fig. 5(b)). The appearance of Li3P indicates
with LPS become looser and rougher (Fig. 4(b)), probably due to the that Li metal reacts with the LPS electrolyte. Similarly, S 2p peak can
reaction between the electrolyte and Li metal. However, the surface be fitted by four different sulfur species shown in Fig. 5(c). The peak
of Li contacted with 1% GO@LPS hybrid SE still remains smooth at 160.8 eV is assigned to Li2S according to reference. [25] The
after cycling for 100 h (Fig. 4(c)), indicating the good protection of detectable Li2S as well as Li3P confirm that the reaction occurs
GO against the interfacial reaction between LPS and Li metal. between Li metal and the LPS electrolyte. The reaction mechanism
Meanwhile, the conductivity changes of the symmetric cells after might follow the equation below:
cycles were also measured as shown in Fig. 4(d) and S4. The
resistance of the pristine cell changes significantly after 10 h’s cycle, Li7P3S11 þ 24 Li / 11 Li2S þ Li3P (2)
indicating the unstable interface between LPS and Li metal. In

Fig. 4. SEM images of (a) as-received Li foil, Li foil assembled with (b) LPS electrolyte after cycling for 20 h and (c) 1% GO@LPS after cycling for 100 h; (d) The resistance of Li/SE/Li
symmetric cell fabricated form LPS and after cycling electrolyte after different cycles at room temperature. (A colour version of this figure can be viewed online.)

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J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

Fig. 5. (a) Schematic diagrams of GO coating to inhibit interfacial reaction between Li and bulk electrolyte. XPS spectra of (b) P 2p and (c) S 2p for LPS, and (d) C 1s, (e) P 2p and (f) S
2p for 1% GO@LPS electrolyte surface after cycling. (A colour version of this figure can be viewed online.)

Fig. 6. (a) Charge-discharge profiles of whole cell assemble from (a) LPS and (b) 1% GO@LPS at 0.05 A g1; (c) CV curves of 1% GO@LPS/graphite batteries at 0.1 mV s1; and (d)
Comparison of the cycling stability of LPS and 1% GO@LPS at 0.05 A g1. (A colour version of this figure can be viewed online.)

When the LPS electrolyte is coated by GO, the C 1s XPS signal components centered at 132.4 (P2S4 3
7 ) and 134.2 eV (PS4 ). The S 2p
(Fig. 5(d)) shows three peaks at 284.0, 284.5 and 289.1 eV, assigned (Fig. 5(f)) peak is fitted into peaks with binding energies of 161.2
to CeO, C]C/CeC and OeC]O bands, respectively. rGO is gener- (PeSeLi) and 161.9 eV (P]S/PeSeP). No peaks for Li2S and Li3P are
ated due to the reaction between Li and GO@LPS as mentioned detected for GO coated LPS, indicating the good protection effect of
afore. However, the P 2p peak (Fig. 5(e)) is fitted into two GO against the interfacial reaction between Li and LPS.

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J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

Fig. 7. (a) The cycling performance of the cell LiCoO2/SEs/Li at 0.1 C; (b) Charge-discharge curves of LiCoO2/SEs/Li cells. (A colour version of this figure can be viewed online.)

Finally, all solid-state graphite/Li battery with SE was assembled electrolyte due to the protection of GO for LPS from the reaction
and the charge-discharge curves at different rates were tested at with Li metal as well as the guidance for the deposition of Li metal.
the room temperature. As exhibited in Fig. 6(a), only one voltage The assembled Li/1% GO@Li7P3S11/Li symmetrical cell can stably
plateau at less than 0.5 V is observed in the first discharge curve of plating/stripping for over 300 cycles at 0.1 mA cm2 at 25  C.
the Li/LPS/graphite battery and it shows an abnormal discharge Coupled with graphite, the full cell exhibits a high initial reversible
capacity (>1700 mAh g1) due to the side reaction and quickly capacity and excellent cycling stability. This facile method not only
broken down after 20 cycles. The charge/discharge profiles of Li/1% deal with the interfacial issues between the Li anode and the sulfide
GO@LPS/graphite cell are shown in Fig. 6(b). The curves overlap solid electrolyte, but also the interfacial issues created between the
well from 10th to 40th cycle, indicating a superior cycling stability Li dendrites within the bulk solid electrolyte, which provides a full
of the all solid-state graphite/Li battery based on the 1% GO@LPS protection for LPS from attack of Li dendrites during cycling. Our
electrolyte. The Liþ storage performance of the cell is investigated study paves the way for addressing the issues of interfacial stability
by the cyclic voltammetry (CV) in the voltage range of 0.01e3 V (vs. between the sulfide solid electrolyte and lithium metal for their
Liþ/Li). Similar CV behaviors in the initial five scans for the full cell application in the all solid state batteries.
with 1% GO@LPS electrolyte are shown in Fig. 6(c). There is a small
peak at about 2.6 V, implying the side reactions between the CRediT authorship contribution statement
graphite and electrolyte. This result is in good agreement with the
previous publication that reported the oxidation of sulfide solid Jianwei Li: Formal analysis, Writing e original draft, Experi-
state electrolyte by electronic percolation pathways in the presence mental design, Materials syntheses, Date analysis, Writing the
of carbon [46e49]. The cycling performance of graphite cathode at original draft preparation. Yuanyuan Li: Formal analysis, Supervi-
50 mA g1 is vividly demonstrated in Fig. 6(d). The discharge ca- sion, Materials syntheses, Date analysis and Supervise Review. Jun
pacity of the cell with LPS is the lower and totally broken after 20 Cheng: Supervision, Writing e review & editing. Qing Sun: Su-
cycles. The 1% GO@LPS electrolyte delivers an initial discharge ca- pervision, Writing e review & editing. Linna Dai: Supervision,
pacity of 350 mAh g1. After 50 cycles, it still remains a specific Writing e review & editing, Supervise Review and Editing.
capacity of 260 mAh g1, corresponding to a 75% capacity retention. Xiangkun Nie: Formal analysis, assisted with date analysis. Lina
This excellent cycling stability is mainly due to the fact that GO Chen: Writing e review & editing. Guifang Han: Writing e review
coating inhibits the Li dendrite growth and the interfacial reaction & editing, Materials characterization and Editing. Lijie Ci: Super-
between the solid electrolyte and Li metal. Fig. 7(a) and b shows the vision, Methodology, Data curation, Conceptualization, Writing e
cycling performances of the Li/LPS/LCO and Li/1% GO@LPS/LCO cell review & editing, Funding acquisition.
at 0.1 C. The initial discharge capacity of Li/1% GO@LPS/LCO cell is
110 mAh g1. After 100 cycles, the discharge capacity still retains
Declaration of competing interest
80 mAh g1 with a capacity retention of 72.7%. In contrast, the bare
Li/LPS/LCO cell only exhibits 2.5 mAh g1 after 100 cycles. With the
The authors declare that they have no known competing
GO coating sulfide solid electrolyte, the Li/1% GO@LPS/LCO cell
financial interests or personal relationships that could have
shows the excellent electrochemical cycle performance, which is
appeared to influence the work reported in this paper.
agree with the results of the symmetrical Li/SE/Li cell test. This
excellent cycling stability is mainly due to the fact that GO coating
inhibits the Li dendrite growth and the interfacial reaction between Acknowledgments
the solid electrolyte and Li metal.
This work was financially supported by High-level Talents’
Discipline Construction Fund of Shandong University (No.
4. Conclusions 31370089963078), Shandong Provincial Science and Technology
Major Project (Nos. 2016GGX104001, 2017CXGC1010, and
In summary, GO and LPS composite solid electrolytes were 2018JMRH0211), the Fundamental Research Funds of Shandong
successfully synthesized using a solution synthesis method. With University (Nos. 2016JC005, 2017JC042 and 2017JC010), the Natural
1% GO addition, the ionic conductivity of the LPS solid electrolyte Science Foundation of Shandong Province (No. ZR2017MEM002),
get increased. Assembled half and whole cells show improved and School Research Startup Expenses of Harbin Institute of Tech-
performance and excellent cycling stability with the 1% GO/LPS nology (Shenzhen) (DD29100027), Financial support from State
58
J. Li, Y. Li, J. Cheng et al. Carbon 177 (2021) 52e59

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