Recent Progress of Single⁃Atom Catalytic Materials for Lithium⁃Sulfur Batteries

doi:10.19894/j.issn.1000-0518.210331

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 513-527.DOI: 10.19894/j.issn.1000-0518.210331

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Recent Progress of Single⁃Atom Catalytic Materials for Lithium⁃Sulfur Batteries

WANG-Xin, ZHANG-Dong(), DU-Fei()

Key Laboratory of Physics and Technology for Advanced Batteries，Ministry of Education，College of Physics，Jilin University，Changchun 130012，China

Received:2021-07-08 Accepted:2021-10-19 Published:2022-04-01 Online:2022-04-19
Contact: ZHANG-Dong, DU-Fei
Supported by:
the National Natural Science Foundation of China(21771086);Jilin Provincial Department of Education “13th Five-Year” Scientific Research Project(JJKH20211034KJ)

Abstract

Abstract:

Lithium-sulfur （Li-S） batteries are one of the promising next-generation energy storage technologies due to their high theoretical specific capacity and energy density. However， in practical applications， low conductivity of sulfur and lithium sulfide， dissolution of polysulfides （LIPSs）， and poor conversion of LIPSs to Li₂S₂/Li₂S result in the short lifespan and low rate performance of Li-S batteries. Recent studies show that single-atoms （SAs） with superior catalytic activities are ideal anchoring centers and catalytic sites for LIPSs. Modification of cathodes and separators with SAs helps to adsorb polysulfide， improve reaction kinetics and inhibit the shuttle effect. In addition， introduction of SAs into the anode can significantly improve the reversibility of Li deposition/stripping and inhibit the growth of dendrites. In this paper， we review the research progress of SAs in lithium-sulfur batteries， including material synthesis， characterization methods， application direction and catalytic mechanism. Finally， the key challenges and future developmental trends of SAs are summarized and discussed.

Key words: Lithium-sulfur batteries, Shuttle effect, Single atom, Polysulfide conversion

CLC Number:

O611

WANG-Xin, ZHANG-Dong, DU-Fei. Recent Progress of Single⁃Atom Catalytic Materials for Lithium⁃Sulfur Batteries[J]. Chinese Journal of Applied Chemistry, 2022, 39(4): 513-527.

Figures/Tables 9

Fig.1 （A） Schematic illustration of the in situ separation and confinement of a platinum precursor in a β-cage followed by thermal treatment［41］；（B） Schematic illustration of the fabrication process of HPC［42］

Fig.2 （A， B） Magnified HAADF-STEM images and （C） energy dispersive X-ray spectroscopy （EDS） elemental mapping results of BiSAs/NC， with C （green）， N （blue）， and Bi （red）［43］；（D） high-resolution XPS N 1s spectra of Co-N/G and N/G ［44］；（E） Schematic illustration of the formation of Fe-SAs/NSC［45］； the normalized XANES spectra and （F） the k3-weighted Fourier transform of EXAFS spectra at Fe K-edge of Fe-SAs/NSC and the reference materials［45］；（G） EXAFS curves between the experimental data and the fit of Fe-SAs/NSC［45］

Fig.3 （A） photograph showing the variation in color of （1） the polysulfide solution after adsorption by （2） PNC and （3） Fe-PNC ［60］；（B） Energy profiles for the sulfur reduction on N-C and Fe-N4-C substrates （the inset in shows the optimized adsorption configurations）［61］； Energy profiles for the dissociation of the Li2S cluster on （C） N-C and （D） Fe-N4-C， The green， yellow， silver and brown balls represent Li， S， N and Fe atoms， respectively［61］；（E） CV curves of Fe-N/MHCS symmetric cells in 0.5 mol/L Li2S6 electrolyte at a scan rate of 1 mV/s［61］；（F） Schematic synthesis illustration of the converted-Li2S nanocomposite with SACo catalyst［62］

Table 1 The electrochemical performance of Li?S batteries using SAs as sulfur hosts

材料 Material	硫负载量 Sulphur load/ （mg·cm^-2）	倍率性能 Rate capability/ （mA?h·g^-1）	电流/循环圈数/容量保持率 Current/number of cycles/ capacity retention rate	参考文献 Ref.
Co-N₄@2D/3D carbon	1	1171 （0.2 C）/695（5 C）	1 C/500/73.5%	［63］
Co?PCNF	1.7	1373.5 （0.2C）/914.3 （2C）	0.5 C/100/95.5%	［64］
Mn/C?（N， O）	1.1	~1100 （0.2 C）/~500 （4 C）	1 C/1000/50%	［65］
FeNSC	1	1193 （0.05 C）/550.2 （4 C）	1 C/1000/53%	［66］
Fe?N/MHCS	2	1110 （0.2 C）/949 （2 C）	1 C/1000/81.3%	［61］
ZnS and Co-N-C DEB sites	9	0.6 C/6.5 mA·h/cm²	0.6 C/100/86.7%	［67］
CoSA?N?C@S	1.2	1574 （0.05 C）/624 （5 C）	1 C/1000/65%	［68］
FeSA?CN	2.4	1123 （0.05 C）/605 （4 C）	4 C/500/70%	［69］
S?SAV@NG	2	1230 （0.2 C）/645 （3 C）	0.5 C/400/70.64%	［70］

Fig.4 （A） CV profiles of the Li-S batteries with unmodified PP， the NG， or M1/NG-modified separators at 0.1 mV/s［71］；（B） Charge-discharge curves of the Li-S batteries at 0.5 C［71］；（C） Voltage gaps of the Li-S batteries with various separators at 600 mA·h/g［71］；（D） CV profiles of the Li-S cell with the Fe1/NG-modified separator， inset： digital photo of the in situ Raman cell； in situ Raman spectra of the Li-S cell with the Fe1/NG-modified separator at different voltages as indicated in （E）［71］

Table 2 The electrochemical performance of Li?S batteries using SAs to modify the separator

材料 Material	硫负载量 Sulphur load/（mg·cm^-2）	倍率性能 Rate capability/（mA·h·g^-1）	电流/循环圈数/容量保持率 Current/number of cycles/capacity retention rate	参考文献 Ref.
W/NG	1.1	1375 （0.2 C）/678 （10 C）	2 C/1000/55%	［74］
NC@SA?Co	1	1160 （0.1 C）/582 （5 C）	2 C/700/59.4%	［73］
Ni@NG	1 mg	1160 （0.1 C）/612 （10 C）	1 C/500/78%	［75］
SC?Co	1.2	~1380 （0.1 C）/680 （3 C）	0.5 C/300/74.2%	［76］
Fe SACs	4.5	1200 （0.2 C）/673 （5 C）	0.5 C/750/83.7%	［71］

Fig.5 （A） Electron density difference and surface binding energy of graphene， ZnSAs， and N-graphene［78］；（B） Li migration pathways and barriers on ZnSAs［78］；（C - D） In situ observation of Li electrodepositing on KB and ZnSAs［78］；（E） Schematic illustration for the Li-S batteries with celgard and B/2D MOF-Co separators［79］；（F - I） SEM images of the initial and cycled Li anodes treated with B/2D MOF-Co［79］

Table 3 The electrochemical performance of Li?S batteries using SAs to modify the anode

材料

Materials

电流密度/电压/循环寿命

Current density （1 mA·cm^-2）/ voltage （mV）/cycle life （h）

锂硫电池的硫负载量

Sulphur Load of lithium?sulfur battery/ （mg·cm^-2）

锂硫电池的电流密度/循环圈数/容量

Current of lithium?sulfur battery /Number of cycles/Capacity（mA?h/g）

参考文献

Ref.

Fig.6 CV curves of the symmetric cells with （A） Li2S6 at a scan rate of 50 mV/s； Potentiostatic discharge profiles of Li2S6 solution at 2.07 V on the CNT substrate using STD-CoPcCl （B） and STD （C） electrolytes；（D） Long-term cycling and （E） rate performance of Li-S batteries［83］

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Recent Progress of Single⁃Atom Catalytic Materials for Lithium⁃Sulfur Batteries

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