A Review on Engineering Transition Metal Compound Catalysts to Accelerate the Redox Kinetics of Sulfur Cathodes for Lithium-Sulfur Batteries

doi:10.1007/s40820-023-01299-9

Abstract

Abstract:

Engineering transition metal compounds (TMCs) catalysts with excellent adsorption-catalytic ability has been one of the most effective strategies to accelerate the redox kinetics of sulfur cathodes. Herein, this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping, bimetallic/bi-anionic TMCs, and TMCs-based heterostructure composites. It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band, d/p-band center, electron filling, and valence state. Moreover, the electronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity, electron filling, and ion radius, resulting in electron redistribution, bonds reconstruction, induced vacancies due to the electronic interaction and changed crystal structure such as lattice spacing and lattice distortion. Different from the aforementioned two strategies, heterostructures are constructed by two types of TMCs with different Fermi energy levels, which causes built-in electric field and electrons transfer through the interface, and induces electron redistribution and arranged local atoms to regulate the electronic structure. Additionally, the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out. It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries.

Key words: Lithium-sulfur battery, Redox kinetic, Transition metal compounds catalyst, Multiple metals/anions

Liping Chen, Guiqiang Cao, Yong Li, Guannan Zu, Ruixian Duan, Yang Bai, Kaiyu Xue, Yonghong Fu, Yunhua Xu, Juan Wang, Xifei Li. A Review on Engineering Transition Metal Compound Catalysts to Accelerate the Redox Kinetics of Sulfur Cathodes for Lithium-Sulfur Batteries[J]. Nano-Micro Letters, 2024, 16(1): 97-.

Liping Chen, Guiqiang Cao, Yong Li, Guannan Zu, Ruixian Duan, Yang Bai, Kaiyu Xue, Yonghong Fu, Yunhua Xu, Juan Wang, Xifei Li. [J]. Nano-Micro Letters, 2024, 16(1): 97-.

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Figures/Tables 11

Fig. 1 a Strategies, b advances of modified transition metal compounds (TMCs) catalysts with multi-cations/anions in LSBs

Fig. 2 a Schematic of in situ etching Mo-doped Ni₃N by LiPSs [44]. Copyright: 2022, Elsevier. b Schematic of evolution of Co-doped MoS₂. c Relationship of the formation energies of 1 T, 2H MoS₂ and doped Co content. d Influence of Co doping on the formation energies of sulfur vacancies in MoS₂. The catalytic effect of Co-doped MoS₂: e Li₂S₄ decomposition and f Li₂S decomposition [45]. Copyright: 2021, American Chemical Society. Effect of Zn doping on the catalytic effect of CoTe₂: g S-S bond length of Li₂S₄ and S-Li bond length of Li₂S. h Gibbs free energies [47]. Copyright: 2022, John Wiley and Sons. Effect of Cu-doped CoP: i unbalanced charge densities induced by Cu doping. j Schematic of electron transfer and variation of bond length, k Comparison of LiPSs/Li₂S conversion barrier [54]. Copyright: 2019, John Wiley and Sons

Fig. 3 Relationship between catalytic activity and adsorption ability: a Schematic of doped ZnS by substituting Zn to tune the electronic structures. b Principle of regulating electronic structure by doping. c Voltage difference and peak current of the CV of symmetric cells. d Relationship of binding energies and d-band center. e Volcano diagram of reaction rates for ZnS doped with different ions (R2: LiPSs dissociation, R3: desorption steps). f Relationship of interactions and catalytic effect [51] Copyright: 2022, Springer Nature

Fig. 4 Superior effect of O-doped NiCo₂(O-S)₄: a sulfidation process NiCo₂(O-S)₄ and NiCo₂S₄. b Ratio of M³⁺/M²⁺ 2p_3/2 peak intensity (I_p) and the rate of I_p change. c NiCo₂(O-S)₄ with high conductivity and LiPSs affinity greatly reserved the catalysis active surface [62]. Copyright: 2022, John Wiley and Sons. Improvement of catalytic effect by N-doped CoSe₂: d PDOS of CoSe₂ and N-CoSe₂. e Charge number of Co in CoSe₂ and N-CoSe₂ [63]. Copyright: 2020, American Chemical Society. P-doped NiTe₂₋_x: f Schematic illustration of P-doped NiTe₂₋_x at Te vacancies. g Difference of Li-Te and S-Ni bond lengths formed between LiPSs and various catalysts. h Charge density difference between Li₂S and catalysts, the yellow (blue) distribution corresponds to charge accumulation (depletion) [65]. Copyright: 2022, John Wiley and Sons

Fig. 5 Co, P co-doped MoS₂: a Schematic illustration of Co, P co-doped MoS₂ (P-Mo_0.9Co_0.1S₂). b HRTEM images of Co, P co-doped MoS₂. c Energy barrier of LiPSs conversion [69]. Copyright: 2019, John Wiley and Sons. Schematic illustration of the functions of different catalysts: d Ni-doped CoSe₂, e Zn-doped CoSe₂, and f Ni/Zn-doped CoSe₂ [55]. Copyright: 2021, John Wiley and Sons

Fig. 6 a Different bonds formed between Li₄Ti₅O₁₂, TiO₂ and LiPSs [83]. Copyright: 2019, Elsevier. b Advantages of Na₂Ti₆O₁₃ array [84]. Copyright: 2021, American Chemical Society. c DOS of Ni/Co phosphides. d Activation energy of Li₂S nucleation on Ni₂P and Ni₂Co₄P₃. e d-band center of Ni₂P and Ni₂Co₄P₃. f COOP diagram of the S1-S2 and S3-S4 bonds of Li₂S₄ [90]. Copyright: John Wiley and Sons. g Schematic diagram of TiO₂ as adsorption material while BaTiO₃ (BT) as electrocatalyst [91]. Copyright: 2020, Elsevier. h Functions of NiMoO₄ for LiPSs [98]. Copyright: 2021, John Wiley and Sons. i Schematic diagram of high-entropy metal oxide (HEMO) for adsorbing LiPSs [110]. Copyright: 2019, Elsevier

Fig. 7 Synergistic catalysis of NiCo-MOF: a Binding energies. b Free energy for the discharging process. c Li₂S decomposition energy barrier. d Calculated DOS. e Co L-edge and Ni L-edge XANES spectra of the MOFs. f Charge density difference of CoNi-MOF [104]. Copyright: 2021, John Wiley and Sons. g Synergistic effect of Zn and Co sites in bimetallic Zn/Co-ZIF MOF [12]. Copyright: 2022, Elsevier. h The strongest interaction obtained for FeCoNi-PBA with the increase in adsorption sites [113]. Copyright: 2021, Elsevier

Fig. 8 a XRD of rGO/MoS₂, rGO/MoSSe and rGO/MoSe₂. b Comparison of binding energies of LiPSs and MoS₂, MoSe₂, MoSSe (V). c DOS states. d, e In situ Raman characterization of cells with rGO/MoS₂ and rGO/MoSSe. f Schematic of rGO/MoSSe as a host for both sulfur and lithium. g Cycling performance at 1C [124]. Copyright: 2022, American Chemical Society

Fig. 9 a Synergistic adsorption and catalysis of CoSe₂/MoS₂ heterostructure for LiPSs. b electron density differences of Li₂S₄ on MoS₂, CoSe₂ and CoSe₂/MoS₂ (the red and green regions represent negative and positive change [137]. Copyright: 2021, John Wiley and Sons. c Comparison of LiPSs conversion and Li₂S precipitation on MoO₂, Mo₂N and MoO₂-Mo₂N [140]. Copyright: 2020, Elsevier. d Binding energies between Fe₃N, Co_5.47N/Fe₃N, Co_5.47N and Li₂S₆ [146]. Copyright: 2022, Elsevier. e Schematic diagram of MoO₃/MoO₂ [147]. Copyright: 2020, Royal Society of Chemistry. f Li₂S growth at the SnO₂-Mo₂N interfaces in 3D model [149]. Copyright: 2021, American Chemical Society

Fig. 10 Band structure of a ZnSe and b CoSe-ZnSe [151]. Copyright: 2021, John Wiley and Sons. c Electron density difference of NiCo-LDH/Co₉S₈ [153]. Copyright: 2020, Elsevier. Energy band of TiN and TiO₂ d before and e after placing in contact [158]. Copyright: 2020, John Wiley and Sons. f DOS of Mo of V-MoN and MoN [159]. Copyright: 2018, John Wiley and Sons. g XPS of Ti 2p peaks of TiO₂/rGO and TiO₂-Ni₃S₂/rGO. h PDOS of Ti and S atom of the Ni₃S₂/TiO₂ interface [164]. Copyright: 2020, John Wiley and Sons. i Schematic diagram of TiN-VN@CNFs used as both Li host and S host to construct full battery [165]. Copyright: 2019, John Wiley and Sons

Table 1 A brief summary of the improvement of cathode performance by different modified TMCs catalysts

Catalysts	Current density (C)	Initial capacities (mAh g⁻¹)	Cycling number	Decay rate (%)	Promoted mechanism	References
Ni-WS₂ WS₂	0.2	1160.8 963.5	100	54.5 55.1	More chemical anchoring sites, enhanced catalytic activity with surface defect	[36]
Ni-MoS₂ MoS₂	0.2	1343.6 1287.8	100	59.5 52.7	Better adsorption ability, increased catalytic activity more active sites	[39]
Ni_0.2Mo_0.8N Mo₂N Ni₃N	1	1280.8 1130 1072	1400 1400 800	36.4 31.7 29.1	Expanded lattice spacing, In situ etching polysulfide and generating vacancies	[40]
Fe(0.1)/Co₃O₄ Fe(0.2)/Co₃O₄ Co₃O₄	0.2	1392.6 - -	150	73.1 53.91 43.13	Multi-shelled structure, rich oxygen-defect	[54]
N/CoSe₂ CoSe₂	0.2	1341 1159	250	68.9 53.1	New defect, closer d-band center, higher charge number of Co, shorter Co-S bonds and weakened S-S and Li-S bonds	[59]
NiSe₂ P-NiSe₂	1	1012.5 931.7	500	72 61.5	Higher electron densities, enhanced electron transfers	[62]
P-NiTe_2-_x NiTe_2-_x NiTe₂	0.2	1309 1270 1207	300	86.2 - -	Bonds reconstruction, electron densities redistribution	[61]
NiCo-LDH-Se-1 NiCo-LDH-Se-2 NiCo-LDH-Se-4	2	- 1332 -	1000	31.6 80.3 74.9	Improved conductivity, optimized electronic structure, abundant active site	[65]
V₂O₅ LiV₃O₈	0.1	1162 1254	100	69.5 77.3	Improved adsorption ability	[81]
TiO₂ BaTiO₃	0.2	913 941	120	79.5 91.2	Self-polarization of BaTiO₃, strong interaction with LiPSs	[87]
Ni₃ZnC_0.7 Ni₃C	1	1275.8 934.6	200	67.4 -	Extra lithiophilic sites of Zn	[90]
HEO CNF	1	879.6 544.2	500	63.5 -	Synergistic effect of multiple cations, abundant active site	[99]
NiCo-MOF Ni-MOF Co-MOF	0.1	974 761 638	80	92 - -	Different catalytic function of Ni and Co, charge redistribution	[12]
FeNi-PBA FeCo-PBA FeCoNi-PBA	0.1	1303.2 1029.4 1234.7	100	15.9 36 36.5	Multi-metal synergistic adsorption	[109]
CoSe₂/MoS₂ CoSe₂ MoS₂	0.1	1425.3 1092.4 1288.4	50	84.6 64.1 67.8	Stronger adsorption ability of CoSe₂, higher catalytic activity of MoS₂	[126]
Ni Ni/Ni₂P Ni₂P	1	721.3 836.1 770	500	60.2 76.1 72.1	Enhanced conductivity, charge transfer, and adsorption	[127]
MoS₂ MoN MoS₂-MoN	0.2	- - 1100	100	64.9 81.4 93.9	Catalyzing LiPSs by MoN, promoting Li⁺ diffusion by MoS₂	[130]
CoSe-ZnSe ZnSe	0.2	1260 -	100	74.8 45.1	Charge redistribution and lattice distortion of heterointerface	[140]
V₈C₇-VO₂ V₈C₇	4	765.3 666.9	900 500	45.1 43.5	Better anchoring ability, lithiophilic nature	[155]
TiO₂/TiN TiO₂	0.3	1397 1177	150	58 59.5	Adsorptive TiO₂, catalytic TiN, charge transfer from TiN to TiO₂	[169]

Table 1 A brief summary of the improvement of cathode performance by different modified TMCs catalysts

Catalysts	Current density (C)	Initial capacities (mAh g⁻¹)	Cycling number	Decay rate (%)	Promoted mechanism	References
Ni-WS₂ WS₂	0.2	1160.8 963.5	100	54.5 55.1	More chemical anchoring sites, enhanced catalytic activity with surface defect	[36]
Ni-MoS₂ MoS₂	0.2	1343.6 1287.8	100	59.5 52.7	Better adsorption ability, increased catalytic activity more active sites	[39]
Ni_0.2Mo_0.8N Mo₂N Ni₃N	1	1280.8 1130 1072	1400 1400 800	36.4 31.7 29.1	Expanded lattice spacing, In situ etching polysulfide and generating vacancies	[40]
Fe(0.1)/Co₃O₄ Fe(0.2)/Co₃O₄ Co₃O₄	0.2	1392.6 - -	150	73.1 53.91 43.13	Multi-shelled structure, rich oxygen-defect	[54]
N/CoSe₂ CoSe₂	0.2	1341 1159	250	68.9 53.1	New defect, closer d-band center, higher charge number of Co, shorter Co-S bonds and weakened S-S and Li-S bonds	[59]
NiSe₂ P-NiSe₂	1	1012.5 931.7	500	72 61.5	Higher electron densities, enhanced electron transfers	[62]
P-NiTe_2-_x NiTe_2-_x NiTe₂	0.2	1309 1270 1207	300	86.2 - -	Bonds reconstruction, electron densities redistribution	[61]
NiCo-LDH-Se-1 NiCo-LDH-Se-2 NiCo-LDH-Se-4	2	- 1332 -	1000	31.6 80.3 74.9	Improved conductivity, optimized electronic structure, abundant active site	[65]
V₂O₅ LiV₃O₈	0.1	1162 1254	100	69.5 77.3	Improved adsorption ability	[81]
TiO₂ BaTiO₃	0.2	913 941	120	79.5 91.2	Self-polarization of BaTiO₃, strong interaction with LiPSs	[87]
Ni₃ZnC_0.7 Ni₃C	1	1275.8 934.6	200	67.4 -	Extra lithiophilic sites of Zn	[90]
HEO CNF	1	879.6 544.2	500	63.5 -	Synergistic effect of multiple cations, abundant active site	[99]
NiCo-MOF Ni-MOF Co-MOF	0.1	974 761 638	80	92 - -	Different catalytic function of Ni and Co, charge redistribution	[12]
FeNi-PBA FeCo-PBA FeCoNi-PBA	0.1	1303.2 1029.4 1234.7	100	15.9 36 36.5	Multi-metal synergistic adsorption	[109]
CoSe₂/MoS₂ CoSe₂ MoS₂	0.1	1425.3 1092.4 1288.4	50	84.6 64.1 67.8	Stronger adsorption ability of CoSe₂, higher catalytic activity of MoS₂	[126]
Ni Ni/Ni₂P Ni₂P	1	721.3 836.1 770	500	60.2 76.1 72.1	Enhanced conductivity, charge transfer, and adsorption	[127]
MoS₂ MoN MoS₂-MoN	0.2	- - 1100	100	64.9 81.4 93.9	Catalyzing LiPSs by MoN, promoting Li⁺ diffusion by MoS₂	[130]
CoSe-ZnSe ZnSe	0.2	1260 -	100	74.8 45.1	Charge redistribution and lattice distortion of heterointerface	[140]
V₈C₇-VO₂ V₈C₇	4	765.3 666.9	900 500	45.1 43.5	Better anchoring ability, lithiophilic nature	[155]
TiO₂/TiN TiO₂	0.3	1397 1177	150	58 59.5	Adsorptive TiO₂, catalytic TiN, charge transfer from TiN to TiO₂	[169]

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