Overcoming Chemical Inertness under Ambient Conditions: A Critical View on Recent Developments in Ammonia Synthesis via Electrochemical N<sub>2</sub> Reduction by Asking Five Questions

Qin, Qing; Oschatz, Martin

doi:10.1002/celc.201901970

Cited by 37 publications

(15 citation statements)

References 119 publications

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“…S4b), indicating a hydrophobic property. This hydrophobicity is expected to be helpful in promoting the ENRR performance by providing strong interaction with N 2 gas [ 48 ].…”

Section: Resultsmentioning

confidence: 99%

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

et al. 2020

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HIGHLIGHTS • The Bi 2 O 3 nanoplates homogeneously decorated free-standing exfoliated graphene (Bi 2 O 3 /FEG) was prepared by a facile electrochemical deposition method. • The Bi 2 O 3 /FEG first used as nitrogen reduction electrocatalyst exhibits excellent electrocatalysis performance and stability for nitrogen reduction reaction in neutral media. • The superior electrocatalytic nitrogen reduction activity is attributed to the strong interaction of the Bi 6p band with the N 2p orbitals, binder-free nature of the electrodes, and facile electron transfer through the graphene nanosheets. ABSTRACT Electrocatalytic nitrogen reduction reaction is a carbonfree and energy-saving strategy for efficient synthesis of ammonia under ambient conditions. Here, we report the synthesis of nanosized Bi 2 O 3 particles grown on functionalized exfoliated graphene (Bi 2 O 3 /FEG) via a facile electrochemical deposition method. The obtained free-standing Bi 2 O 3 /FEG achieves a high Faradaic efficiency of 11.2% and a large NH 3 yield of 4.21 ± 0.14 μg NH 3 h −1 cm −2 at − 0.5 V versus reversible hydrogen

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“…S4b), indicating a hydrophobic property. This hydrophobicity is expected to be helpful in promoting the ENRR performance by providing strong interaction with N 2 gas [ 48 ].…”

Section: Resultsmentioning

confidence: 99%

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

et al. 2020

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“…Besides, the graphene nanosheets in RuO 2 À Bi 2 O 3 /FEG enable a facile electron, and the hydrophobic property of RuO 2 À Bi 2 O 3 /FEG provides a strong interaction with N 2 gas, further accelerating the NRR process (Figure 4d). [61,62] Subsequently, to explore the NRR electrocatalytic activity of the RuO 2 À Bi 2 O 3 /FEG hybrid in strong basic and acidic media, chronoamperometry tests were conducted in N 2 -saturated 0.1 M KOH and 0.05 M H 2 SO 4 electrolyte under the same experimental conditions as that of in Na 2 SO 4 electrolyte. The LSV curves of RuO 2 À Bi 2 O 3 /FEG shown in Figure S8 (Supporting Information) indicate that RuO 2 À Bi 2 O 3 /FEG can effectively catalyze the NRR both in 0.1 M KOH and 0.05 M H 2 SO 4 .…”

Section: Electrochemical Nitrogen Reductionmentioning

confidence: 99%

Synergy of Bi₂O₃ and RuO₂ Nanocatalysts for Low‐Overpotential and Wide pH‐Window Electrochemical Ammonia Synthesis

Yu²,

Deng

et al. 2021

Chemistry A European J

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Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is still seriously impeded by the inferior NH 3 yield and low Faradaic efficiency, especially at low overpotentials. Herein, we report the synthesis of nanosized RuO 2 and Bi 2 O 3 particles grown on functionalized exfoliated graphene (FEG) through in situ electrodeposition, denoted as RuO 2 À Bi 2 O 3 /FEG. The prepared self-supporting RuO 2 À Bi 2 O 3 /FEG hybrid with a Bi mass loading of 0.70 wt% and Ru mass loading of 0.04 wt% shows excellent NRR performance at low overpotentials in acidic, neutral and alkaline electrolytes. It achieves a large NH 3 yield of 4.58 � 0.16 μg NH3 h À 1 cm À 2 with a high Faradaic efficiency of 14.6 % at À 0.2 V versus reversible hydrogen electrode in 0.1 M Na 2 SO 4 electrolyte. This performance benefits from the synergistic effect between Bi 2 O 3 and RuO 2 which respectively have a fairly strong interaction of Bi 6p orbitals with the N 2p band and abundant supply of *H, as well as the binder-free characteristic and the convenient electron transfer via graphene nanosheets. This work highlights a new electrocatalyst design strategy that combines transition and maingroup metal elements, which may provide some inspirations for designing low-cost and high-performance NRR electrocatalysts in the future.

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“…Ammonia (NH 3 ) is one of the most important chemical products in modern society. [1][2][3][4][5][6] The annual output of NH 3 in the world exceeds 200 million tons. [7] NH 3 as nitrogen fertilizer is an essential for grain production, and can also be used as a carbon-free energy carrier, which can be easily transported in liquid form.…”

Section: Introductionmentioning

confidence: 99%

Cerium Zirconium Solid Solution with High Faradaic Efficiency for Electrochemical Nitrogen Reduction Reaction under Ambient Condition

et al. 2021

ChemElectroChem

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Industrial synthesis of ammonia (NH 3 ) involves high energy consumption resulting in intense pollution. Alternatively, electrochemical nitrogen reduction reaction (NRR) to NH 3 can be carried out under mild conditions, which is a new green NH 3 synthesis method. Herein, cerium zirconium solid solutions (Zr x Ce 1-x O 2 ) with different proportions were synthesized by NH 3 precipitation method and employed as electrocatalysts for NRR. The performance of the different catalysts in 0.1 mol L À 1 Na 2 SO 4 was evaluated with H 2 O and N 2 as reactants. The results show that Zr 0.9 Ce 0.1 O 2 has the highest Faraday efficiency (FE) of 62.68 % at À 1.3 V (vs. Ag/AgCl) and the highest yield rate of NH 3 À 9.34 × 10 À 11 mol cm À 2 s À 1 at À 1.35 V (vs. Ag/AgCl). The impressive FE is due to more oxygen vacancies in Zr 0.9 Ce 0.1 O 2 introduced by Ce 3 + , which is more prone to the adsorption of N 2 on the catalyst surface and facilitates the electrochemical reaction.

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Overcoming Chemical Inertness under Ambient Conditions: A Critical View on Recent Developments in Ammonia Synthesis via Electrochemical N₂ Reduction by Asking Five Questions

Cited by 37 publications

References 119 publications

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Synergy of Bi₂O₃ and RuO₂ Nanocatalysts for Low‐Overpotential and Wide pH‐Window Electrochemical Ammonia Synthesis

Cerium Zirconium Solid Solution with High Faradaic Efficiency for Electrochemical Nitrogen Reduction Reaction under Ambient Condition

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Overcoming Chemical Inertness under Ambient Conditions: A Critical View on Recent Developments in Ammonia Synthesis via Electrochemical N2 Reduction by Asking Five Questions

Cited by 37 publications

References 119 publications

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Synergy of Bi2O3 and RuO2 Nanocatalysts for Low‐Overpotential and Wide pH‐Window Electrochemical Ammonia Synthesis

Cerium Zirconium Solid Solution with High Faradaic Efficiency for Electrochemical Nitrogen Reduction Reaction under Ambient Condition

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Overcoming Chemical Inertness under Ambient Conditions: A Critical View on Recent Developments in Ammonia Synthesis via Electrochemical N₂ Reduction by Asking Five Questions

Synergy of Bi₂O₃ and RuO₂ Nanocatalysts for Low‐Overpotential and Wide pH‐Window Electrochemical Ammonia Synthesis