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Progress in Chemistry 2020, Vol. 32 Issue (1): 33-45 DOI: 10.7536/PC190606 Previous Articles   Next Articles

Special Issue: 电化学有机合成

Electroreduction of Nitrogen to Ammonia Catalyzed by Non-Noble Metal Catalysts under Ambient Conditions

Fenya Guo1, Hongwei Li1, Mengzhe Zhou2, Zhengqi Xu2, Yueqing Zheng1, Tingting Li1,**()   

  1. 1. Chemistry Institute for Synthesis and Green Application, School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, China
    2. Medical School, Ningbo University, Ningbo 315211, China
  • Received: Online: Published:
  • Contact: Tingting Li
  • About author:
    ** E-mail:
  • Supported by:
    National Natural Science Foundation of China(21603110)
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Ammonia is an important chemical for producing fertilizer and also an important carbon-free energy carrier. Haber-Bosch process is the main method to synthesize ammonia. However, it suffers from some severe problems, such as the high energy consumption, the massive emission of greenhouse gas CO2 and the poor catalytic efficiency. Recently, ammonia synthesis based on electrocatalytic nitrogen reduction reaction (NRR) by using renewable energy under mild reaction conditions has attracted wide research attention. In addition, the raw materials (N2 + H2O) are earth abundant. Although great advances have been achieved in electrocatalytic NRR field, some challenges including the high-cost of noble metal based electrocatalysts, the low ammonia yield and unsatisfactory Faradaic efficiency, as well as the unexplored catalytic mechanism of NRR still exist. In this review, we summarize the recent advances in electrocatalytic NRR field based on heterogeneous catalysts. Firstly, we discuss the catalytic thermodynamics and reaction mechanisms towards NRR. Secondly, a range of recently reported non-noble metal included catalysts are surveyed, including transition metal oxides/nitrides/sulfides, metal-free materials and single-metal-atom catalysts. Then, some promising strategies to enhance the catalytic activity, selectivity and efficiency are proposed, and the main methods for the determination of ammonia are also mentioned. Finally, the challenges remaining to be solved are summarized, and future perspectives are also presented.

Key words: electrochemical ammonia synthesis, non-noble metal catalysts, catalytic mechanism, catalyst optimization, determination of ammonia
Fig. 1 The mechanism of electrochemical N2 reduction reaction based on heterogeneous catalysts[10]
Fig. 2 (a) The HR-TEM image of Cr2O3 microspheres; (b) The i~t plots obtained from different applied potentials; (c) The corresponding UV-Vis spectra obtained after long-term tests; (d) The durability test for Cr2O3 microspheres[56]
Fig. 3 (a) The SEM image of VN nanoparticles; (b) The electrocatalytic NRR performance; (c) The electrocatalytic mechanism and corresponding deactivation pathway[63]
Fig. 4 (a) SEM image for defect-rich MoS2 nanoflower; (b) The corresponding UV-Vis spectra obtained after long-term tests; (c) The corresponding NH3 yields under different potentials; (d) Calculated free energy profile for NRR process on MoS2 basal plane[67]
Fig. 5 (a) Schematic illustration of NRR over B-doped graphene; (b) Percentages of different B doping configurations in three B-doped graphene samples; (c) The Faradaic efficiency values of BG-1, BOG, BG-2 and G at different applied potentials[76]
Fig. 6 (a) Scheme of the synthetic procedure for Ru/N-C; (b~e) Comparison of electrocatalytic NRR performance for Ru/N-C and Ru nanoparticles[84]
Fig. 7 (a) Atomic level surface structures of Au THH NR; (b) Geometric models of an Au THH NR and exposed {730} facet; (c) Schematic for electrocatalytic NRR; (d) Yield rate of ammonia, hydrazine hydrate formation, and Faradic efficiency at each given potential[91]
Fig. 8 (a) Schematic for electrocatalytic NRR based on MoN nanosheet array; (b) The corresponding SEM image; (c,d) The electrocatalytic performance under various applied potential[92]
Fig. 9 (a) The SEM image for BCN materials; (b) Schematic of the computational models. Gray (black), pink, red, blue, and green balls represent C, B, O, N, and H atoms, respectively; (c) The corresponding electrocatalytic NRR performance based on different catalysts[97]
Table 1 Summary of recently reported NRR electrocatalysts
Catalyst Electrolyte NH3 yield rate Faraday efficiency(%) Ref
Noble metalcatalyst Au nanocage 0.5 M LiClO4 3.9 μg·h-1·cm-2 (-0.5 V vs. RHE) 30.2 25
Au nanorod 0.1 M KOH 1.648 μg·h-1·cm-2 (-0.2 V vs. RHE) 4 91
Ru/C 2 M KOH 0.21 μg·h-1·cm-2 (-1.1 V vs. Ag/AgCl) 0.28 27
RuPt/C 18.36 μg·h-1·cm-2 (0.123 V vs. RHE) 13.2 28
Rh ultrathin nanosheet 0.1 M KOH 23.88 μg·h-1·m g cat - 1 (-0.2 V vs. RHE) 0.217 31
Pt/C H+/Li+/N H 4 + 47.2 μg·h-1·cm-2 (1.2 V) 0.83 32
Non-noble metal catalyst Fe2O3/CNT dilute KHCO3 solution 0.22 μg·h-1·cm-2 (-0.2 V vs. Ag/AgCl) 0.15 49
Fe2O3-rGO 0.5 M LiClO4 22.13 μg·h-1·m g cat - 1 (-0.50 V vs. RHE) 5.89 51
Fe2O3- x /CNT 0.1 M KOH 0.46 μg·h-1·cm-2 (-0.9 V vs. Ag/AgCl) 6.0 52
Fe3O4/Ti 0.1 M Na2SO4 5.6×10-11 mol·s-1·cm-2 (-0.4 V vs. RHE) 2.6 53
Hollow Cr2O3 mircometer
ball		 0.1 M Na2SO4 25.3 μg·h-1·m g cat - 1 (-0.9 V vs. RHE) 6.78 56
Mo2N 0.1 M HCl 78.4 μg·h-1·m g cat - 1 (-0.3 V vs. RHE) 4.5 62
VN 0.05 M H2SO4 20.2 μg·h-1·cm-2 (-0.1 V vs. RHE) 6 63
MoS2 0.1 M Na2SO4 8.08×10-11 mol·s-1·cm-2 (-0.5 V vs. RHE) 1.17 66
Defect-rich MoS2 nanoflower 0.1 M Na2SO4 29.28 μg·h-1·m g cat - 1 (-0.4 V vs. RHE) 8.34 67
MoS2/graphene 0.1 M LiClO4 24.82 μg·h-1·m g cat - 1 (-0.45 V vs. RHE) 4.58 68
CoS x /NS-G 0.05 M H2SO4 25.0 μg·h-1·m g cat - 1 (-0.2 V vs. RHE) 25.9
(-0.05 V vs.RHE)		 69
MoN nanosheet array 0.1 M HCl 3.01×10-10 mol·s-1·cm-2 (-0.3 V vs. RHE) 1.15 92
Bi nanosheet array 0.1 M HCl 6.89 × 10-11 mol·s-1·cm-2 (-0.5 V vs. RHE) 10.26 93
Bi4V2O11/CeO2 0.1 M HCl 23.21 μg·h-1·mg-1 (-0.2 V vs. RHE) 10.16 96
Metal-free catalyst Oxidized carbonnanotube 0.1 M LiClO4 32.33 μg·h-1·m g cat - 1 (-0.4 V vs. RHE) 12.50 73
N-doped Carbon 0.1 M KOH 3.4×10-6 mol·h-1·cm-2(-0.4 V vs. RHE) 10.2 75
B-doped graphene 0.05 M H2SO4 9.8 μg·h-1·cm-2 (-0.5 V vs. RHE) 10.8 76
N, P-codoped porous carbon 0.1 M HCl 0.97 μg·h-1·m g cat - 1 (-0.2 V vs. RHE) 4.2 77
BCN 0.1 M HCl 7.75 μg·h-1·mgcat.-1 (-0.2 V vs. RHE) 13.79 97
nitrogen-decifient polymeric carbon nitride 0.1 M HCl 8.09 μg·h-1·m g cat - 1 (-0.2 V vs. RHE) 11.59 98
S-CNS 0.1 M Na2SO4 19.07 μg·h-1·m g cat - 1 (-0.7 V vs. RHE) 7.47 99
single metal atom catalyst Au/C3N4 0.05 M H2SO4 1.3 mg·h-1·m g Au - 1 (-0.1 V vs. RHE) 11.1 83
Ru/N-C 0.05 M H2SO4 120.9 μg·h-1·mg-1 (-0.2 V vs. RHE) 29.6 84
Ru/N-C 0.1 M HCl 3.665 m g N H 3 ·h-1·m g Ru - 1 (-0.21 V) 21 (-0.11 V) 85
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