Research Progress of Controlling Lithium-Sulfur Batteries by Electrocatalysts under Lean Electrolyte Conditions

doi:10.19894/j.issn.1000-0518.220175

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (2): 188-209.DOI: 10.19894/j.issn.1000-0518.220175

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Research Progress of Controlling Lithium-Sulfur Batteries by Electrocatalysts under Lean Electrolyte Conditions

Lu-Fei WANG¹, Meng-Meng ZHEN¹(), Bo-Xiong SHEN²()

^1.School of Energy and Environmental Engineering，Hebei University of Technology，Tianjin 300071，China
^2.School of Chemical Engineering and Technology，Hebei University of Technology，Tianjin 300071，China

Received:2022-05-10 Accepted:2022-08-04 Published:2023-02-01 Online:2023-02-27
Contact: Meng-Meng ZHEN,Bo-Xiong SHEN
About author:shenbx@hebut.edu.cn
zhenmengmeng@hebut.edu.cn；
Supported by:
the National Natural Science Foundation of China(51702236);the Natural Science Foundation of Hebei Province(B2021202052)

Abstract

Abstract:

Lithium-sulfur batteries （LSBs） have high theoretical energy density （2600 Wh/kg） and high theoretical specific capacity （1675 mA·h/g） and are regarded as one of the most promising electrochemical energy storage systems to replace lithium-ion batteries for commercial applications. However， the inherent slow redox kinetics and the “shuttle effect” of lithium polysulfides （LiPSs） seriously affect cycle performances of LSBs. At present， most of the reviews focus on the design of sulfur host materials for LSBs under excess electrolyte， researches on improvement of battery performances under lean electrolyte are less. Herein， this paper introduces the regulation of different electrocatalysts on the redox reaction kinetics of LSBs under lean electrolytes. It is mainly divided into two categories： non-metallic catalysts （non-metallic compounds， graphene， carbon nanotubes and heteroatom doped carbon materials） and metal catalysts （cobalt-based， molybdenum-based， iron-based and multi-metal-based heterogeneous structures）. Finally， further researches are proposed and prospected to promote the commercial application of LSBs.

Key words: High energy density, Lean electrolyte, Electrocatalysts, Reaction kinetics, Lithium-sulfur battery performances

CLC Number:

O611

Lu-Fei WANG, Meng-Meng ZHEN, Bo-Xiong SHEN. Research Progress of Controlling Lithium-Sulfur Batteries by Electrocatalysts under Lean Electrolyte Conditions[J]. Chinese Journal of Applied Chemistry, 2023, 40(2): 188-209.

Figures/Tables 21

Fig.1 （A） Typical charge-discharge curves for non-aqueous LSBs［14］；（B） Illustration of the catalytic mechanism during charge-discharge process in LSBs［15］

Fig.2 （A） Transmission electron microscopy （TEM） image of black phosphorus （BP） that is centrifuged at 4000 r/min；（B） TEM image of BP centrifuged at 8000 r/min （BP-8K）；（C） High-resolution TEM （HRTEM） image and corresponding selected area electron diffraction （SAED） pattern （inset） of BP-8K；（D-F） TEM and HRTEM images of BPQDs；（G） Raman spectra of bulk BP （red） and BPQD （blue） on a silicon （Si） substrate；（H） Initial discharge-charge profiles at 0.1 C between 1.7 and 2.8 V vs.Li+/Li；（I） Cyclic performance of the PCNF/S/BPQD at 0.1 C for 200 cycles；（porous carbon nanofibers，PCNFs）［47］

Fig.3 （A） Schematic illustration of the synthesis process of porous carbon@borocarbonitride （KB@BCN）；（B） SEM and （C） TEM images of KB@BCN-2；（D） Optical photographs of an adsorption experiment between Li2S6 solution （0.003 mol/L） and KB@BCN-2 or KB；（E） Cycle performance of KB@BCN-2-S at 0.2 C with a low E/S=5 μL/mg［53］

Fig.4 （A） Low-magnification S and （B） high-magnification SEM images of CGCC；（C） SEM images of CGCC cathode；（D） SEM images of cycled CGCC cathodes；（E） Illustration of the synthesis route of the CGCC cathode；（F） Cyclability performance of CGCC cathodes［49］

Fig.5 （A） Schematic and digital images of the CNT paper and the Li2S6-CNT electrode； SEM images of （B） the CNT paper and （C， D） the Li2S6-CNT electrode from the top （c） and the bottom （d）； Energy density of the Li||Li2S6-CNT full cells shown in （E） and （F）［56］

Fig.6 （A） Schematic of the fabrication process of a CNT aerogel@Li2S8 cathode；（B） Digital photo of a CNT aerogel；（C， D） SEM images of a CNT aerogel@Li2S8 cathode；（E） CNT aerogel@Li2S8 cathode with high S loading area specific capacity at 0.2 C；（F） Voltage profiles of different cathodes；（G） Areal specific capacities of the CNT aerogel@Li2S8 cathodes with high S loadings compared to commercial LIBs；（H） Charge and discharge curves of a CNT aerogel@Li2S8 pouch cell at 0.1 C［57］

Fig.7 SEM images of （A） NCNFs and （B） VNCNFs；（C） and （D） TEM images of VNCNFs；（E） Schematic illustration of the synthetic process of asymmetric bifunctional VNCNFs membrane and diagram of the S/VNCNFs||VNCNFs/Li full cell configuration；（F） The long-term cycle life of the S/VNCNFs||VNCNFs/Li full cell with a sulfur load of 8.3 mg/cm2；（G） The areal capacity of the S/VNCNFs||VNCNFs/Li full cell with a high sulfur load of 15.27?mg/cm2 at 1 mA/cm2. （Li-S， lithium-sulfur； PECVD， plasma-enhanced chemical vapor deposition； SEM， scanning electron microscopy）［60］

Fig.8 （A） Schematic illustration of the synthesis process of S@WLC-CNTs electrodes；（B-D） SEM images of the WLC-CNTs host；（E） SEM image of the S@WLC-CNTs cathode with sulfur loading of 17.3 mg/cm2；（F-G） Cyclability of S@WLC-CNTs electrodes with different thicknesses and sulfur content at the 0.1 C［62］

Table 1 The electrochemical performance of nonmetallic catalysts in LSB under lean electrolyte

Material	E/S ratio （μL·mg^-1）	Sulfur loading/ （mg·cm^-2）	Current/number of cycles	Discharge capacity/ （mA·h·g^-1）	Area capacity/ （mA·h·cm^-2）	Ref.
PCNF/S/BPQDs	6.5	8.0	0.1 C/200	550	4.4	［47］
KB@BCN-2-S	5.0	4.0	0.2 C/100	677	2.7	［53］
CGCC	4.2	57.6	0.1 C/200	539	31.0	［49］
HCFF-S	3.53	21.2	3.55 （mA/cm²）/150	698	14.8	［54］
CNTaerogel@Li₂S₈	7.8	20.0	0.2 C/70	535	10.7	［57］
S/NF@VG	4.8	13.0	0.1 C/100	846	~11	［59］
S/VNCNFs\|\|VNCNFs/Li	4.0	15.27	1.0 （mA/cm²）/50	851	13.0	［60］
S@WLC-CNTs	6.0	52.4	0.1 C/100	692	36.2	［62］

Fig.9 （A） Voltage profiles and （B） cycling trend at the constant current rate of C/20 of the Li|S∶Au 97∶3（m/m） cell with sulfur loading over the electrode of 5.7 mg/cm2 and E/S ratio of 5 μL/mg［67］；（C） Preparation procedure of Co-NC@TpBD-Me2 cathode and its working mechanism as sulfur cathode；（D） Cycling of S/Co-NC@TpBD-Me2 cathode at 0.2 C under high sulfur loadings［69］

Fig.10 （A） Design strategy of macroporous host with DEB sites；（B） Optimized configurations of Li2S4， Li2S6 and Li2S8 absorption on ZnS （a1-a3）， the Co-N-C surface （b1-b4） and the ZnS， Co-N-C surface （c1-c4）； The yellow， pink， silver， brown， blue and cyan balls denote the S， Li， Zn， Co， N and C atoms， respectively； The 3D ordered macroporous sulfur host with ZnS and Co-N-C DEB sites （“3d-omsh/ZnS，Co-N-C”）［71］

Fig.11 （A） Schematic diagrams of the synthetic procedure of Co-NCNT@CF/S；（B） Cycling performance of Co-NCNT@CF/S electrode under different E/S ratios at 0.1?C；（C） The cycling performance of the Co-NCNT@CF/S cathode at 0.1 C；（D） Initial charge-discharge profiles of different electrodes with a 0.1?C current rate；（E） Values of ΔH and QL/QH calculated from the charge/discharge curves［73］；（F） Schematic illustration of the synthesis of CNT-CoP-Vp；（G） STEM-HADDF image of CNT-CoP-Vp-1M， the insert image is the theoretical model of CoP；（H） The intensity of Co and P atomic columns along blue dotted line in （G）［75］

Fig.12 （A） Schematic Illustration of the Fabrication of rGO-CNT-CoP（A） and rGO-CNT-CoP（C） Composite；（B， C） TEM， HRTEM images of rGO-CNT-CoP（A）；（D， E） TEM， HRTEM images of rGO-CNT-CoP（C）；（F） Binding energies of Li2S6， Li2S4， and Li2S on rGO-CNT-CoP （A） and rGO-CNT-CoP （C）；（G） Density of states of d bands of Co and p bands of P［76］；（H） Schematic of the synthesis route for S/CoSe@C and CoSe@C/Li；（I） Cycling stability of the S/CoSe@C||CoSe@ C/Li cell at 0.2 C rate；（J） Cycling stability of the S/CoSe@C||CoSe@C/Li cell at 0.1 C rate. Nitrilotriacetic acid （NTC）［78］

Fig.13 （A） Schematic illustration of the advantages of Li2S-Co9S8/Co in LSBs；（B） Cycling stability of the Li2S-Co9S8/Co cathode at 1 C rate；（C） Cycling stability of the Li2S-Co9S8/Co cathode with various Li2S loadings at 0.1 C rate；（D） Cycling stability of the Li2S-Co9S8/Co-Te cathode in the Ni||Li2S pouch cell［81］

Fig.14 （A） Schematic diagram of the fabrication process of MoB；（B， C） Low-magnification TEM images of MoB；（D） HRTEM images of MoB；（E） Schematic illustration of the advantages of catalytic electrode in LSBs；（F） Cycling stability of the MoB/S cathode in coin cell at 0.2 C rate；（G） A comparative cycling stability of the MoB/S and C/S cathodes in pouch cells with an E/S ratio of 4.5 μL/mg and a sulfur loading of 3.5 mg/cm2 at C/20 rate［82］

Fig.15 （A） Synthesis processes of the schematic illustration of the Co-MoSe2/MXene；（B-D） Electrochemical performance of S/Co-MoSe 2 /MXene monolith cathodes in lean electrolyte at 0.1 C，（B） Long-term cycling stability at the E/S ratio of 5.0 μL/mg；（C） Gravimetric and volumetric capacities and （D） areal capacities at an E/S ratio of 3.5 μL/mg［90］

Fig.16 （A） FeF2@rGO synthetic route diagram；（B） XRD patterns of FeF2@rGO；（C） Schematic diagram of the cathode catalytic conversion process during cycle；（D） Cycling performances of FeF2@rGO cathode and rGO cathode under high sulfur loading at 0.1 C［96］

Fig.17 （A） Schematic illustration for the synthesis of Fe2O3/N-MC， N-MC and their application in LSBs；（B） SEM image and （C） TEM image and （D， E） HRTEM images of S@Fe2O3/N-MC；（F） The short cycling performance of S@Fe2O3/N-MC cathode under different E/S ratio and sulfur loading and （G） long-term cycling performance under high areal loading （5.1 and 6.5 mg/cm2） at 1.0 C［97］

Fig.18 （A） Catalytic mechanism and （B） SEM image and （C） HRTEM image of Nb4N5-Nb2O5 heterostructures；（D） Optimized geometries and their corresponding binding energies of Li2S4 on Nb4N5 （211） and Nb2O5 （001） surfaces；（E） Schematic configuration of Nb4N5-Nb2O5 heterostructures based full batteries；（F） Areal capacity of Nb4N5-Nb2O5/Li||Nb4N5-Nb2O5/S battery obtained at 0.3 C with high sulfur loading of 6.9 mg/cm2 and （G） Cycling performance of the full battery operated at an elevated temperature of 50 ℃［100］

Fig.19 （A） The working principle of the Li-S full battery based on the “two-in-one” ZnSe-CoSe2@NC hosts；（B） SEM images of ZnSe-CoSe2@NC；（C） XRD pattern of ZnSe-CoSe2@NC， CoSe2@NC and ZnSe@NC；（D） Cycle performance of the full cell under high sulfur loading and lean electrolyte［101］；（E） Schematic illustration of MoS2， MoS2-MoN， and MoN nanosheets grown on nitrogen-doped carbon nanotube （NCNT） vertically； SEM images of （F） MoS2，（G） MoS2-MoN and （H） MoN hosts；（I） Galvanostatic charge/discharge curves for different E/S ratios with sulfur loadings of 12.2 mg/cm2；（J） Cycling performances of MoS2-MoN/S cathodes with sulfur loadings of 12.2 mg/cm2 with different E/S ratios at 0.1 C for 100 cycles；（K） Cycling performance of MoS2-MoN/S cathode at 0.5 C for 200 cycles［102］

Table 2 Electrochemical performance of metal catalysts for LSB under lean electrolyte

Material	E/S ratio/ （μL·mg^－1）	Sulfur loading/ （mg·cm^－2）	Current/number of cycles	Discharge capacity/ （mA·h·g^－1）	Area capacity/ （mA·h·cm^－2）	Ref.
m（S）∶m（Au）=97∶3	5.0	5.7	0.05 C/40	730	4.2	［67］
S/Co-NC@TpBD-Me₂	6.1	5.71	0.2 C/50	793	4.53	［69］
ZnS and Co-N-C DEB sites	4.0	6.25	83.33 （mA/g）/80	1 257	7.86	［71］
Co-NCNT@CF/S	3.9	8.8	0.1 C/100	579	5.10	［73］
S/CNT-CoP-Vp	5.0	7.7	0.4 （mA/cm²）/30	1 043	8.03	［75］
S/rGO-CNT-CoP（A）	7.0	5.3	0.8 （mA/cm²）/50	833	4.43	［76］
S/CoSe@C\|\|CoSe@C/Li	4.5	6.2	0.1 C/100	680	4.2	［78］
N-CoSe₂/S	4.4	10.2	0.2 C/70	~790	~8.1	［80］
Li₂S-Co₉S₈/Co	5.0	8.3（Li₂S）	0.1 C/150	653	-	［81］
MoB/S	7.0	6.1	0.2 C/200	647	3.95	［82］
MoS_2－_x /rGO	5.0	5.6	0.5 （mA/cm²）/100	730	4.1	［86］
S/Co-MoSe₂/MXene	3.5	9.9	0.1 C/50	606	~6.0	［90］
FeNC/wG	7.8	5.39	0.5 C/50	776	4.18	［92］
FeHCF-A	5.6	5.2	0.2 C/180	865	4.5	［93］
FeF₂@rGO/S	6.0	12.73	0.1 C/50	882	11.2	［96］
S@Fe₂O₃/N-MC	5.7	6.5	1.0 C/200	745	4.84	［97］
CoSe-ZnSe@G	3.0	7.7	0.01 C/40	532	4.1	［98］
Nb₄N₅-Nb₂O₅	5.1	6.9	0.3 C/200	725	5.0	［100］
ZnSe-CoSe₂@NC	4.1	6.08	0.2 C/100	642	4.16	［101］
MoS₂-MoN	4.2	12.2	0.1 C/78	893	10.9	［102］

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Research Progress of Controlling Lithium-Sulfur Batteries by Electrocatalysts under Lean Electrolyte Conditions

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