金属单原子催化剂增强硫正极动力学的研究进展

doi:10.3866/PKU.WHXB202212005

Abstract

Abstract:

Sulfur has been considered as an ideal cathode of lithium sulfur batteries (LSBs) owing to its high theoretical energy density (2600 Wh∙Kg^-1), excellent discharge capacity (1672 mAh∙g^-1), and low cost. During sulfur reduction and oxidation processes, nevertheless, the sluggish redox reaction kinetics of the sulfur cathode and severe shuttle effect of soluble lithium polysulfides intermediates significantly result in poor battery performance. It has been demonstrated that a sulfur host with high adsorption energy and excellent catalytic activity/selectivity can effectively enhance the cycle stability and rate capability of LSBs. As a result, a variety of hosts, such as metal compounds, heterojunctions, defect matrices, and single metal atom catalysts, have been widely developed. Interestingly, single metal atom catalysts with a unique electronic structure, low metal content, theoretical 100% atom utilization efficiency, and high catalytic performance can effectively promote the conversion of different lithium polysulfides intermediates and provide abundant absorption sites for sulfur-contained species, thereby optimizing the redox reaction kinetics of the sulfur cathode and shuttle behavior of the soluble lithium polysulfides. Various single metal atom catalysts, mainly including iron, cobalt, nickel, zinc, tungsten, vanadium, molybdenum, and manganese, have been developed via atomic bonding, spatial confinement, and defect engineering strategies to solve the key challenges of sulfur cathode since single metal atom catalysts were for the first time to be utilized as catalytic agents for LSBs. In this review, the interaction among support materials in single metal atom catalysts, atomically dispersed metal catalytic sites, and the sulfur cathode were addressed in detail, providing a basis for the development of high-performance single metal atom catalysts. Furthermore, advanced characterization techniques such as in situ Raman spectroscopy, X-ray absorption spectroscopy, cyclic voltammograms, and electrochemical impedance spectroscopy, were employed to investigate the catalytic effect of single metal atom catalysts. Notably, the effects of the coordination environment on the catalytic activity and selectivity of single metal atom catalysts were systematically discussed. Simultaneously, the catalytic mechanism of single metal atom catalysts with different metal/nonmetallic atoms and coordination configurations was elucidated using theoretical calculations. In addition, some significant challenges of single metal atom catalyst in LSBs were proposed. It is believed that this review will provide a novel insight into the optimization of atomic catalysts with high activity and catalytic selectivity toward long-lifespan LSBs.

Key words: Sulfur cathode, Reaction kinetics, Single metal atom catalyst, Polysulfide conversion, Lithium sulfur battery

Jingjing Wang, Guiqiang Cao, Ruixian Duan, Xiangyang Li, Xifei Li. Advances in Single Metal Atom Catalysts Enhancing Kinetics of Sulfur Cathode[J]. Acta Phys. -Chim. Sin. 2023, 39(5), 2212005. doi: 10.3866/PKU.WHXB202212005

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Host Material	Sulfur Loading (w/%)	Rate/C	Cycle number	Reversible Capacity/(mAh∙g⁻¹)	Decay rate per cycle/%	Ref.
Fe-PNC	70	0.1	300	427	0.2	47
FeSA-CN	68.7	4.0	500	N/A	0.06	55
Co-N/G	90	1.0	500	681	0.053	26
SAFe@g-C₃N₄	N/A	2.0	1000	624	0.03	96
NC: SAFe	N/A	5.0	1000	315	0.06	97
CoSA-N-C	74.2	1.0	1000	675	0.035	58
Co-PCNF	N/A	1.0	800	549.7	0.054	46
FeN₂ -NC	~75	1.0	500	800	0.055	64
Fe-N₂/CN	69.5	2.0	2000	620	0.011	82
Mo-N-C	81	2.0	550	~800	0.018	83
Mo-N-CNF	72	1.0	400	714	0.062	54
Fe-N₅-C	74	1.0	500	662	N/A	27
3DFeSA-CN	82.9	1.0	2000	N/A	0.031	48
Fe SAs@BCN	N/A	5.0	1000	593	0.018	98
FeSA-PN@PNC	N/A	1.0	800	N/A	0.04	89
Mn/C-(N, O)	76	1.0	1000	N/A	0.05	28
Ni−N₅/HNPC	80	0.5	500	798	0.053	50
SAV@NG	80	0.5	400	551	0.073	61
FeNSC	65	1.0	1000	477.1	0.047	90
MoSe₂@rGO	75.8	1.0	270	823	N/A	99
1T’-MoSe₂	N/A	0.33	250	N/A	0.15	18
MnO₂@HCF	71	0.5	300	662	N/A	100
Ti₄O₇	70	0.5	100	N/A	N/A	101
WO@NC	< 60	2.0	1200	N/A	0.038	102
RuO_2−x	67	1.0	600	602	0.08	103
VS₂@G/CNT	N/A	0.5	300	701	N/A	104
VN/G	N/A	1.0	200	917	0.09	105

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Advances in Single Metal Atom Catalysts Enhancing Kinetics of Sulfur Cathode

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