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Progress in Chemistry 2021, Vol. 33 Issue (7): 1074-1091 DOI: 10.7536/PC200714 Previous Articles   Next Articles

• Review •

Electrocatalytic Nitrogen Reduction Reaction under Ambient Condition: Current Status, Challenges, and Perspectives

Xiaolu Liu1, Yuxiao Geng1, Ran Hao1, Yuping Liu1,*(), Zhongyong Yuan2, Wei Li1   

  1. 1 Key Laboratory of Advanced Energy Materials Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China
    2 National Institute for Advanced Materials, School of Materials Science and Engineering, Nankai University, Tianjin 300350, China
  • Received: Revised: Online: Published:
  • Contact: Yuping Liu
  • About author:
    * Corresponding author e-mail:
  • Supported by:
    National Natural Science Foundation of China(21421001); National Natural Science Foundation of China(21573115); National Natural Science Foundation of China(21875118)
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Ammonia (NH3) is one of the most important nitrogen-based fertilizers and chemicals, and is also a novel hydrogen storage material. It is made on an industrial scale via the Haber-Bosch process, which requires high temperature and high pressure to consume a large amount of energy. It is very urgent to find an environmentally benign alternative process to alleviate the crises for energy and environment. Electrocatalytic nitrogen reduction reaction (NRR) has attracted worldwide research interest. However, such process is actually hard to perform due to the inherent inertness of N2 molecules together with the low solubility in aqueous solutions. Although great research efforts have been made to explore and design suitable electrocatalysts for ammonia synthesis, the yield of ammonia is still very low. In addition, the ambiguous mechanism still remains as a major barrier for the development of NRR systems. In this review, we firstly introduced the catalytic reaction mechanisms towards NRR. Then we overviewed of the latest progress of the state-of-art catalysts in the electrocatalytic NRR. Moreover, we put more emphasis on the various rational strategies for electrocatalyst design to enhance the NRR performance, such as size effects, facets regulation, defects engineering, amorphization, which are aiming to increasing the exposed active sites or altering the electronic structure to further improve the apparent or intrinsic activity. Finally, we briefly discussed the main challenges in this field. We hope this review will offer a helpful guidance for the reasonable design of electrocatalysts towards NRR, arouse more interests in the new research field of NRR, and promote the green ammonia synthesis industrialization as soon as possible.

Contents

1 Introduction

2 NRR Mechanisms

3 The factors of electrocatalytic NRR system

3.1 Modified reactor configuration

3.2 Suitable applied potential

3.3 Effects of electrolytes

4 Research progress of electrocatalyst of NRR

4.1 Noble metal-based electrocatalysts

4.2 Non-noble metal-based electrocatalysts

4.3 Metal-free electrocatalysts

4.4 Single-metal-atom electrocatalysts

5 Electrocatalysts design for NRR

5.1 Size effects

5.2 Defect engineering

5.3 Morphology effects

5.4 Amorphous phases

6 Conclusion and outlook

Key words: nitrogen reduction reaction, electrocatalysis, ammonia synthesis, catalyst design, ambient condition
Scheme 1 Schematic depiction of (a) the dissociative pathway, (b) associative alternating pathways, (c) associative distal associative for catalytic conversion of N2 to NH3[4], Copyright 2020, Wiley-VCH
Fig.1 Schematics of different cell configurations of (a) PEM-type cell, (b) Single chamber and (c) H-type cell for NRR at ambient conditions[3]. Copyright 2018, Wiley-VCH
Fig. 2 (a) Transmission electron microscopy image of Au THH NRs and the geometric model. (b) NH3 yield rates and FEs at each given potential. (c) Setup of the electrolytic cell used for the NRR. (d) Free energy diagram and catalytic pathway of N2 reduction on the Au THH NRs[37]. Copyright 2017, Wiley-VCH
Fig. 3 (a) NH3 synthesis Faradic efficiency and (b) corresponding yield rate. (c) NRR catalytic mechanism of the Mo2C/C under proton-suppressed and proton-enriched condtions[79]. Copyright 2019, Wiley-VCH
Fig. 4 (a) HAADF-STEM image of Pt SAs/WO3. (b) HRTEM image of Pt NPs/WO3. (c) Yield of NH3 and Faradaic efficiency of Pt SAs/WO3 and Pt NPs/WO3. (d) Electrochemical in situ time-resolved Fourier transform infrared (FT-IR) spectra for nitrogen reduction reaction (NRR) on the Pt SAs/WO3 electrode[94]. Copyright 2020, Wiley-VCH.
Fig. 5 (a) Schematic diagram of Al-Co3O4/NF synthesis. (b, c) SEM images of Al-Co3O4/NF. (d) The proposed limitation and promotion of NRR behavior from different surface interface structures. (e) Electrochemical in situ-FTIR spectra of NRR on Al-Co3O4/NF. (f) Corresponding possible pathway for NH3 production[115]. Copyright 2020, ACS
Table 1 Summary of recently reported NRR electrocatalysts.
Catalyst Electrolyte NH3 yield rate FE (%) Potential
(V vs RHE)		 ref
Noble metal-
based materials		 THH Au nanorods 0.1 mol/L KOH 1.648 μg·h -1·c m - 2 4.0 -0.2 37
Hollow Au nocages 0.5mol/L LiClO4 3.9 μg·h -1·c m - 2 30.2 -0.5 120
porous Au film 0.1 mol/L Na2SO4 9.42 μg·h -1·c m - 2 13.36 -0.2 38
Au/TiO2 0.1mol/L HCl 21.4 μg·h -1 m g cat. - 1 8.11 -0.2 99
a-Au/CeOx-rGO 0.1 mol/L HCl 8.3 μg·h -1 m g cat. - 1 10.1 -0.2 127
Pd/C 0.1mol/L PBS 4.5 μg·h -1 m g cat. - 1 8.2 0.1 27
Pd0.2Cu0.8/rGO 0.1 mol/L KOH 2.80 μg·h -1 m g cat. - 1 17.8 -0.2 48
Pt93Ir7alloy 0.001 mol/L HCl 28 μg·h -1·c m - 2 40.8 -0.3 34
Rh nanosheet 0.1 mol/L KOH 23.88μg·h-1·m g cat. - 1 0.217 -0.2 54
Ag nanosheets 0.1 mol/L HCl 4.62×10-11mol ·s -1·cm-2 4.8 -0.6 44
Ag3Cu networks 0.1 mol/L Na2SO4 24.59 μg·h -1 m g cat. - 1 13.28 -0.5 47
Non-noble metal-
based materials		 Fe2O3nanorode 0.1mol/L Na2SO4 15.9 μg·h -1 m g cat. - 1 0.94 -0.8 22
Fe/Fe3O4 0.1mol/L PBS 0.19 μg·h -1·c m - 2 8.29 -0.3 57
MoO3 0.1 mol/L HCl 4.80×10-10 mol·s-1·cm-2 1.9 -0.5 59
Nb2O5 nanofiber 0.1 mol/L HCl 43.6 μg·h -1 m g cat. - 1 9.26 -0.55 61
NbO2 0.05 mol/L H2SO4 11.6 μg·h -1 m g cat. - 1 32 -0.65 60
Mn3O4 NP@rGO 0.1 mol/L Na2SO4 17.4 μg·h -1 m g cat. - 1 3.52 -0.85 62
r-WO3nanosheets 0.1 mol/L HCl 17.28 μg·h -1 m g cat. - 1 7 -0.3 63
WO3-x nanosheets 0.1 mol/L HCl 4.2 μg·h -1 m g cat. - 1 6.8 -0.12 64
Bi4V2O11/CeO2 0.1 mol/L HCl 23.21 μg·h -1 m g cat. - 1 10.16 -0.2 126
Ti3C2Tx MXene N.A. 0.26 μg·h -1·c m - 2 5.78 -0.2 103
Mo2C/C 0.5mol/L H2SO4 11.3 μg·h -1 m g cat. - 1 7.8 -0.2 79
MoS2 nanoflower 0.1mol/L Na2SO4 29.28 μg·h -1 m g cat. - 1 8.34 -0.4 107
Mo2N 0.1 mol/L HCl 78.4 μg·h -1 m g cat. - 1 4.5 -0.3 73
MoN NA/CC 0.1 mol/L HCl 3.01×10-10 mol·s-1·cm-2 1.15 -0.3 74
W2N3 nanosheets 0.1 mol/L KOH 11.66±0.98 μg·h-1 m g cat. - 1 11.67 ± 0.93 -0.2 76
Metal-free materials N-doped carbon 0.1 mol/L KOH 57.8 μg·h -1 cm-2 10.2 -0.3 118
PCN 0.1 mol/L HCl 8.09 μg·h -1 m g cat. - 1 11.59 -0.2 106
B-doped graphene 0.05 mol/L H2SO4 9.8 μg·h -1·c m - 2 10.8 -0.5 84
B4C 0.1 mol/L HCl 26.57 μg·h -1 m g cat. - 1 15.95 -0.75 88
Single atom
metal materials		 Ru SAs/N-C 0.05 mol/L H2SO4 120.9 μg·h -1 m g cat. - 1 29.6 -0.2 92
Ru@ZrO2/NC 0.1 mol/L HCl 3665 μg·h -1 m g cat. - 1 21 -0.21 93
Au1/C3N4 0.005 mol/L H2SO4 1305 μg·h -1 m g cat. - 1 11.1 -0.1 V vs Ag/AgCl 91
Pt SAs/WO3 0.1 mol/L K2SO4 342.4 μg·h -1·m g Pt - 1 31.1 -0.2 94
Mo SAs/N-C 0.1 mol/L KOH 34.0±3.6 μg·h-1·m g cat. - 1 14.6±1.6 -0.3 95
Fe SAs/MoS2 0.1 mol/L KCl 97.5±6 μg·h-1·c m - 2 31.6±2 -0.2 96
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