Two-dimensional Transition Metal Dichalcogenides for Electrocatalytic Oxygen Reduction Reaction

doi:10.15541/jim20220128

Abstract

Abstract:

Oxygen reduction reaction (ORR) is the key reaction in cathode for fuel cells. Because of the sluggish kinetics, platinum (Pt) is widely used as the electrocatalysts for ORR. However, the high cost of Pt and poor stability of carbon black support under high voltage limit the commercialization and durability of fuel cells. Two-dimensional transition metal dichalcogenides (2D TMDs) possess large specific area, tunable electronic structure, and high chemical stability, making them a good candidate for ORR catalysts with high activity and durability. This paper reviews the recent progress of 2D TMDs-based ORR electrocatalysts. First, crystal structure, electronic properties, and ORR reaction mechanism are briefly introduced. Then some strategies for adjusting ORR performance of 2D TMDs are summarized, including heteroatom doping, phase conversion, defect engineering, and strain engineering. Meanwhile, the ORR activity enhancement arising from 2D TMDs-based heterostructures is also analyzed. Finally, perspectives are given for current issues and their possible solutions.

Key words: oxygen reduction reaction, two-dimensional material, transition metal dichalcogenide, electrocatalysis, review

CLC Number:

O614

SUN Lian, GU Quanchao, YANG Yaping, WANG Honglei, YU Jinshan, ZHOU Xingui. Two-dimensional Transition Metal Dichalcogenides for Electrocatalytic Oxygen Reduction Reaction[J]. Journal of Inorganic Materials, 2022, 37(7): 697-709.

Figures/Tables 11

Fig. 1 Structures and crystal forms of 2D TMDs

Fig. 2 Calculated band structures of (a) bulk MoS2, (b) quadrilayer MoS2, (c) bilayer MoS2, and (d) monolayer MoS2[26]

Fig. 3 Designing strategy for ORR catalysts[3,41] (a) ORR mechanism with blue arrow representing dissociative mechanism, red arrows representing associative mechanism, and purple arrows representing the parts involving both mechanisms[3]; (b) “Volcano plots” showing relationship between oxygen binding energy and maximal activity[41] Colorful figures are available on website

Table 1 Properties of typical 2D TMDs-based ORR catalysts

Catalyst	Electrolyte	Onset potential / V (vs. RHE)	Half-wave potential / V (vs. RHE)	Electrons transfer number, n	Ref.
P-MoS₂-0.2	0.1 mol·L^-1 KOH	0.96	0.80	3.60	[45]
I-PdSe₂-50	0.1 mol·L^-1 KOH	-	0.76	3.67	[46]
Ag/MoS₂	0.1 mol·L^-1 KOH	0.90	0.83	3.98	[47]
2H+1T-FeSe@NC	1.0 mol·L^-1 KOH	0.97	0.80	3.90	[48]
O-MoS₂-87	0.1 mol·L^-1 KOH	0.94	0.80	3.49	[49]

Fig. 4 M-position doping for 2D TMDs[53,55] (a) ORR energy barrier for Pt-MoSe2 with insets showing crystal structures[53] ; (b) TEM images of Pt-SAs/2D TMDs prepared by galvanic replacement[55]

Fig. 5 X-position doping of 2D TMDs[45,61] (a) ORR polarization curves of P-MoS2 in 0.1 mol·L-1 KOH[45]; (b) Corresponding possible reaction mechanism[61]

Fig. 6 (a) Preparative schematic illustration by phase conversion from 2H-MoS2, (b) ORR polarization curves in 0.1 mol·L-1 KOH, and (c) corresponding K-L plots of 1T-MoS2[68] Colorful figures are available on website

Fig. 7 Defect and strain engineering of 2D TMDs[46,49,65] (a) TEM images and (b) O1s XPS spectra of defected I-PdSe2[46]; (c) Schematic illustration of synthesis of O-MoS2 (d) ORR polarization curves in 0.1 mol·L-1 KOH of O-MoS2[49]; (e) AFM (left) and TEM (middle and right) images of 2H-1T WS2 showing the formation of strain[65]

Table 2 Properties of typical 2D TMDs heterostructures-based ORR catalysts

Catalyst	Electrolyte	Onset potential / V (vs. RHE)	Half-wave potential / V (vs. RHE)	Electrons transfer number, n	Ref.
Pt/MoS₂-rGO	0.1 mol·L^-1 HClO₄	0.90	0.80	-	[85]
MoS₂-CNT	0.1 mol·L^-1 KOH	0.65	-	~4.00	[86]
MoS₂/S-PC	0.5 mol·L^-1 H₂SO₄	-	0.86	4.00	[87]
Ni₃S₂/MoS₂	0.1 mol·L^-1 KOH	0.95	0.88	3.99	[88]
hBN-MoS₂	0.1 mol·L^-1 KOH	0.80	0.60	4.00	[89]
FePc-MoS₂	0.1 mol·L^-1 KOH	-	0.89	4.00	[90]

Fig. 8 2D TMDs@carbon materials heterostructure ORR catalysts[85,92] (a) TEM images and (b) activity variations of Pt/MoS2-rGO[85]; (c) SEM image and (d) power density of microbial fuel cells based on N-MoS2/C catalysts[92] Colorful figures are available on website

Fig. 9 Other 2D TMDs-based heterostructure ORR catalysts[88⇓-90] (a) TEM image of Ni3S2/MoS2 and (b) corresponding ORR polarization curves in 0.1 mol·L-1 KOH[88]; (c) TEM image of hBN/MoS2 and its (d) ORR durability test[89]; (e) Structure of FePc-MoS2 and (f) its integrated partial density of states IPDOS[90]

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