Electro-synthesis of ammonia from nitrogen at ambient temperature and pressure in ionic liquids

Zhou, Fengling; Azofra, Luis Miguel; Ali, Muataz; Kar, Mega; Simonov, Alexandr N.; McDonnell-Worth, Ciaran James; Sun, Chenghua; Zhang, Xinyi; MacFarlane, Douglas R.

doi:10.1039/c7ee02716h

Cited by 548 publications

(494 citation statements)

References 43 publications

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“…Notably,i fa ll this extra increased reduction current is used for the NRR under the N 2 -saturated environment (Figure 3a), the NH 3 yield rate at À0.3 Vversus RHE is calculated to be 119.6 mg NH 3 h À1 mg cat. [40][41][42] Moreover, 1 HNMR spectroscopy with isotope-labeled 15 N 2 [43] confirms that the ammonia detected in the NRR experiments was produced from the NRR ( Figure S17). À1 ).…”

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confidence: 58%

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

et al. 2019

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NH 3 synthesis by the electrocatalytic N 2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method-the Haber-Boschp rocess-that requires high temperature and pressure.W er eport single Mo atoms anchored to nitrogendoped porous carbon as ac ost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks,t his catalyst achieves ah igh NH 3 yield rate (34.0 AE 3.6 mg NH 3 h À1 mg cat. À1 )a nd ahigh Faradaic efficiency (14.6 AE 1.6 %) in 0.1m KOHatroom temperature.T hese values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover,t his catalyst displays no obvious current drop during a5 0000 sN RR, and high activity and durability are achieved in 0.1m HCl. The findings provideapromising lead for the design of efficient and robust single-atom non-preciousmetal catalysts for the electrocatalytic NRR.

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confidence: 58%

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

et al. 2019

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“…[42] Figure 2a shows the UV-vis absorption spectra of various electrolytes colored with indophenol indicator after electrocatalytic reaction for 3 h at different potentials ranging from −0.29 to −0.59 V ( Figure S7, Supporting Information). [43] Figure S10a and desorption on MnO/TM. Furthermore, NH 3 yields and FEs at various potentials ( Figure S9, Supporting Information) determined by ion chromatography data (Table S1, Supporting Information) are quite comparable to the values obtained from the indophenol blue method.…”

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Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

et al. 2018

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NH3 is a valuable chemical with a wide range of applications, but the conventional Haber–Bosch process for industrial‐scale NH3 production is highly energy‐intensive with serious greenhouse gas emission. Electrochemical reduction offers an environmentally benign and sustainable route to convert N2 to NH3 at ambient conditions, but its efficiency depends greatly on identifying earth‐abundant catalysts with high activity for the N2 reduction reaction. Here, it is reported that MnO particles act as a highly active catalyst for electrocatalytic hydrogenation of N2 to NH3 with excellent selectivity. In 0.1 m Na2SO4, this catalyst achieves a high Faradaic efficiency up to 8.02% and a NH3 yield of 1.11 × 10−10 mol s−1 cm−2 at −0.39 V versus reversible hydrogen electrode, with great electrochemical and structural stability. On the basis of density functional theory calculations, MnO (200) surface has a smaller adsorption energy toward N than that of H with the *N2 → *N2H transformation being the potential‐determining step in the nitrogen reduction reaction.

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“…Considering these aspects, the following alternative tactics have been proposed. First, mixed electrolytes or ionic liquid electrolytes with trace water instead of aqueous electrolytes have been employed to limit the proton concentration and its transfer rate on the electrocatalyst surface . Additionally, the concentration and acidity of proton donors can be fine‐tuned.…”

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confidence: 99%

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

et al. 2020

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Ammonia (NH3) is a pivotal precursor in fertilizer production and a potential energy carrier. Currently, ammonia production worldwide relies on the traditional Haber–Bosch process, which consumes massive energy and has a large carbon footprint. Recently, electrochemical dinitrogen reduction to ammonia under ambient conditions has attracted considerable interest owing to its advantages of flexibility and environmental friendliness. However, the biggest challenge in dinitrogen electroreduction, i.e., the low efficiency and selectivity caused by poor specificity of electrocatalysts/electrolytic systems, still needs to be overcome. Although substantial progress has been made in recent years, acquiring most available electrocatalysts still relies on low efficiency trial‐and‐error methods. It is thus imperative to establish some critical guiding principles for nitrogen electroreduction toward a rational design and accelerated development of this field. Herein, a basic understanding of dinitrogen electroreduction processes and the inherent relationships between adsorbates and catalysts from fundamental theory are described, followed by an outline of the crucial principles for designing efficient electrocatalysts/electrocatalytic systems derived from a systematic evaluation of the latest significant achievements. Finally, the future research directions and prospects of this field are given, with a special emphasis on the opportunities available by following the guiding principles.

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Electro-synthesis of ammonia from nitrogen at ambient temperature and pressure in ionic liquids

Abstract: High faradaic efficiency reduction of N2 to NH3 is achieved in ionic liquid media under ambient conditions.

Cited by 548 publications

References 43 publications

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

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Electro-synthesis of ammonia from nitrogen at ambient temperature and pressure in ionic liquids

Abstract: High faradaic efficiency reduction of N2 to NH3 is achieved in ionic liquid media under ambient conditions.

Cited by 548 publications

References 43 publications

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Electrocatalytic Hydrogenation of N2to NH3by MnO: Experimental and Theoretical Investigations

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

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Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations