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Progress in Chemistry 2021, Vol. 33 Issue (12): 2392-2403 DOI: 10.7536/PC201109 Previous Articles   Next Articles

• Review •

Single-Atom-Modified MoS2 for Efficient Hydrogen Evolution

Jiaqi Han, Zhida Li, Deqiang Ji, Dandan Yuan, Hongjun Wu()   

  1. College of Chemistry & Chemical Engineering, Northeast Petroleum University,Daqing 163318, China
  • Received: Revised: Online: Published:
  • Contact: Hongjun Wu
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The over-reliance on fossil fuels leads to deteriorating ecological environment and motivates us to develop sustainable and clean energy alternatives in order for our long-term survival on the earth. Hydrogen energy is one of the most promising energy carriers in the 21st century since the only by-product is H2O. In comparison to steam reforming of natural gas and coal, hydrogen evolution reaction (HER) via H2O electrolysis is a more attracting pathway for H2 production because of the low cost, high efficiency and abundant raw materials, which would contribute to a lower carbon footprint. HER requires stable and active enough catalyst materials to overcome the reaction barriers. It is well known that Pt group materials are state-of-the-art HER catalysts, but unfortunately, the low abundance and high cost complicate its large-scale applications. The transition metal disulfides (TMDs) possess a two-dimensional layered structure and a larger specific surface area, which is conducive to expose more active sites. In particular, MoS2, a representative of TMDs, has attracted tremendous research interests in HER domain and is supposed to be a cost-affordable alternative to Pt-based catalysts. In this work, the research status of MoS2 modified by single atoms (SA-MoS2) of noble metal, non-noble metal, and nonmetal, to catalyze HER reactions is reviewed. Based on the overpotential and Tafel slope, the structure-function relationship between HER performance and SA-MoS2 structures is summarized. Finally, future research directions are proposed and hopefully, this paper will guide rational design of SA-MoS2 for a more efficient HER electrocatalyst.

Contents

1 Introduction

2 Metal single-atom doped MoS2

2.1 Noble metal elements platinum (Pt), palladium (Pd), ruthenium (Ru), tungsten (W)

2.2 Transition metal elements nickel (Ni), cobalt (Co), copper (Cu)

3 Non-metal single-atom doped MoS2

4 Conclusion and outlook

Key words: hydrogen evolution, molybdenum disulfide, single atom, electrocatalysis
Fig.1 The hydrogen evolution mechanism of MoS2 nanoflowers in 0.5 mol·L-1 H2SO4[43]. Reproduced from Ref. 43 with permission from the Centre National de la Recherche Scientifique (CNRS) and The Royal Society of Chemistry.
Fig.2 Phase diagrams of MoS4[53]
Table 1 MoS2 electrocatalysts modified with noble metal single atoms
Atom Electrolyte Initial potential(mV) Overpotentialηj(mV) Tafel slope(mV/dec) ref
Pt 0.1 mol/L H2SO4 - η10≈140 96 61
Pd 0.5 mol/L H2SO4 - η10=78 72 62
Ru 1 mol/L KOH - η10=76 21 63
W 0.5 mol/L H2SO4 -37 η10=138 55 64
Fig.3 TEM and HAADF-STEM images of Pt-MoS2(a) TEM image of Pt-MoS2; (b) the single Pt atoms (marked by red circles) uniformly disperse on the 2D MoS2 plane; (c) a honeycomb arrangement of MoS2 and the amplificatory image[61].Reproduced from Ref. 61 with permission from the Centre National de la Recherche Scientifique (CNRS) and The Royal Society of Chemistry
Fig.4 EDX mappings of Pt-MoS2 (a) HAADF-STEM image of Pt-MoS2; (b~d) EDX mappings of Mo, S and Pt[61]
Fig.5 HER performance of Pt-MoS2 (a) polarization curves; (b) Tafel plots[61]
Fig.6 Schematic illustration of the spontaneous MoS2/Pd (Ⅱ) redox reaction[62]
Fig.7 HAADF-STEM images of (a) MoS2, (b) 1%Pd-MoS2[62]
Fig.8 HER performance of Pd-MoS2 electrocatalysts (a) polarization curves, (b) Tafel plots[62]
Fig.9 (a,c) HAADF-STEM images of SA-Ru-MoS2; (b,d) Magnified domains of the orange dashed rectangles shown in (a) and (c)[63]
Fig.10 Schematic diagram of the generation of S vacancies caused by Ru single atom doping[63]
Fig.11 HER catalytic performance of Ru-MoS2(a) LSV polarization curves; (b) Tafel plots[63]
Fig.12 HER activity of Mo1-xWxS2(a) polarization curves, (b) corresponding Tafel plots[64]
Fig.13 HAADF-STEM image of Mo0.5W0.5S2[64]
Table 2 MoS2 electrocatalysts modified with transition metal single atoms
atom Electrolyte Initial potential(mV) Overpotaenial ηj(mV) Tafel slope(mV/dec) ref
Ni 0.5 mol/L H2SO4 - η10=110 74 65
Ni 1 mol/L KOH - η10=98 75 65
Co 0.5 mol/L H2SO4 220 - 92 66
Cu 0.5 mol/L H2SO4 - η10=131 51 68
Fig.14 HER activity of NiO@1T-MoS2(a) Polarization curves; (b) Tafel plots[70]
Fig.15 (a,b) HAADF-STEM image of Co-MoS2; (c,d) Atomic structure diagram, yellow, green and red balls represent S, Mo and Co[66].Reproduced from Ref. 70 with permission from the Centre National de la Recherche Scientifique (CNRS) and The Royal Society of Chemistry
Fig.16 HER activity of SA Co-D 1T MoS2 (a) Polarization curves; (b) Tafel plots[72]
Table 3 MoS2 electrocatalysts modified with non-metal single atoms
Atom Electrolyte Initial potential(mV) Overpotential ηj(mV) Tafel slope(mV/dec) ref
N 0.5 mol/L H2SO4 35 η100=121 41 75
O 0.5 mol/L H2SO4 120 - 55 76
P 0.5 mol/L H2SO4 15 η10≈43 34 77
Se 0.5 mol/L H2SO4 ≈-140 - 55 79
Fig.17 TEM and HRTEM images of N-MoS2-3[75]
Fig.18 EDX mapping of N-MoS2-3[75]
Fig.19 HER activity of N-MoS2(a) polarization curves ; (b)Tafel plots ; (c) polarization curves for N-MoS2-3 before and after 5000 CV cycles ; (d)The theoretical and experimental amount of hydrogen produced by the sample N-MoS2-3 as a function of time for 60 min[75]
Fig.20 XPS spectra A: high-resolution Mo 3d; B: high-resolution S 2p ; C: high-resolution O 1s[76]
Fig.21 HER activity of the oxygen-incorporated MoS2 ultrathin nanosheets A: polarization curves ; B: Tafel plots[76]
Table 4 Tafel slopes of MoS2 prepared under different temperatures[76]
Sample Temp( ℃) Tafel slopemV/dec
S140 140 67
S160 160 58
S180 180 55
S200 200 63
Fig.22 Atomic structure diagram of P-doped MoS2[77]
Fig.23 (a) SEM image of P-doped MoS2 (b) TEM image of P-doped MoS2[77]
Fig.24 HER activity of P-MoS2 (a) Polarization curves ; (b) Tafel plots ; (c) Electrochemical impedance spectra of different electrodes at -0.25 V versus RHE; (d) Plot of charge transport resistance of P-MoS2-1, P-MoS2-2, MoS2[78].Reproduced from Ref. 78 and Ref. 79 with permission from the Centre National de la Recherche Scientifique (CNRS) and The Royal Society of Chemistry
Fig.25 Schematic illustration of preparing Se-doped MoS2 nanosheets[79]
Fig.26 HER activity of Se-doped MoS2 nanosheets (a)Polarization curves; (b)Tafel plots[79]
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