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Progress in Chemistry 2020, Vol. 32 Issue (5): 505-518 DOI: 10.7536/PC190938   Next Articles

Special Issue: 电化学有机合成

• Review •

Synthesis, Characterization and Analysis of Graphene-Supported Single-Atom Catalysts

Jianlei Qi, Qinqin Xu, Jianfei Sun, Dan Zhou, Jianzhong Yin**   

  • Revised: Online: Published:
  • Contact: Jianzhong Yin
  • About author:
    ** e-mail:
  • Supported by:
    National Natural Science Foundation of China(U1662130); National Natural Science Foundation of China(21978043)
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Single-atom catalyst has the advantages of low coordination number, special coordination environment, high atomic utilization, and high uniformity of catalytic sites. It is the bridge between homogeneous and heterogeneous catalysts, which helps to better understand the nature of catalytic reaction. In this paper, the synthetic methods of graphene-based single-atom catalysts in recent years are reviewed, including atomic layer deposition, impregnation-calcination, defect trapping, coordination anchoring and some other novel methods, with a focus on the preparation process, principle and characterization results of these methods. Based on this, the performance of graphene-based metal single-atom catalysts in catalysis is illustrated and analyzed, and the purpose is to provide guidance and reference for the preparation of single-atom catalysts.

Contents

1 Introduction

2 Synthetic method

2.1 Atomic layer deposition method

2.2 Impregnation-calcination method

2.3 Defect trapping method

2.4 Coordination anchoring method

2.5 Other methods

3 Performance evaluation and characterization

3.1 Hydrogen evolution reaction

3.2 Carbon dioxide reduction reaction

3.3 Oxidation reaction

3.4 Hydrogenation reaction

4 Conclusion and outlook

Key words: single-atom, catalyst, graphene, performance and characterization, preparation
Table 1 The related parameters of Pt loading with different cycle times
Carrier Cycle index Partical
size(nm)		 Loading
(wt%)		 ref
rGO 50 0.5 1.52 42
100 1~2 2.67 42
150 2~4 10.5 42
N-doped graphene 50 - 2.1 45
100 - 7.6 45
Fig. 1 (a) HAADF-STEM images of Pt atom clusters[42];(b) HAADF-STEM images of Pd atom[49];(c) HAADF-STEM images of Pt diatomics[51];(d) schematic diagram of single atom prepared by atomic layer deposition[52]
Fig. 2 (a) HAADF-STEM images of Co-NG[24];(b) schematic of the synthesis process of the Fe/NG catalyst[62];(c) the Ni-NG/CdS composite materials[26];(d) EDX elemental mapping of Ni-NG within the selected area[26]
Fig. 3 (a) The mass production of catalyst[65];(b) Schematic illustration of preparation route to Co-NG-MW[66]
Fig. 4 (a) Schematic illustration of the fabrication process of Ni-doped np-G[76];(b) HAADF-STEM image of Ni-doped graphene[76];(c) synthetic route towards single-atom FeN4 and FeN5 catalysts[79]
Fig. 5 (a) LSV of NG, Co-G, Co-NG and Pt/C in 0.5 M H2SO4 at scan rate of 2 mV·s-1[24];(b) Gibbs free energy of HER at equilibrium potential for different materials[76];(c) illustration of Pt atoms configurations on N-doped graphene[45];(d) XPS spectra of materials at different dissolution times[76]
Table 2 Overpotential of hydrogen evolution reaction with different catalysts
Catalyst Electrolyte Overpotential of
10 mA/cm2		 ref
Co-NG 0.5 M H2SO4 147 24
Co-NG-MW 0.5 M H2SO4 175 66
Ni-doped np-G 0.5 M H2SO4 180 76
ALD50Pt/NGNs 0.5 M H2SO4 <50 45
A-Ni@NG 0.5 M H2SO4 70 32
Pt/C 0.5 M H2SO4 50~70 32, 66, 76
Fig. 6 (a) Photocatalytic hydrogen production rate over Ni-NG/CdS, Pt/CdS, NG/CdS and bare CdS under visible light irradiation[26];(b) catalytic activities of various Pt catalysts in AB hydrolysis[51]
Fig. 7 (a) LSV of Ni-N-MEGO, NiPc, N-MEGO and MEGO in CO2 saturated 0.5 M KHCO3 solution[63];(b) theoretical calculations and proposed mechanism on the nitrogen-coordinated Fe catalytic site[62]
Fig. 8 Faradaic efficiencies for formate at each applied potentials and TOF of the catalyst[65]
Fig. 9 (a) The XANES spectra at Pt L3 edge of Pt foil, Pt/C, ALD150Pt/GNS, Pt/GNS, ALD100Pt/GNS, ALD50Pt/GNS[42];(b) schematic illustration of improvement of butenes selectivity on single atom Pd1/graphene catalyst[49];(c) durability test for the Pd1/N-graphene catalyst for over 24 h at 125 ℃[67]
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