How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully

Tang, Cheng; Qiao, Shi Zhang

doi:10.1039/c9cs00280d

Cited by 804 publications

(584 citation statements)

References 48 publications

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“…Nitrogen, as one of the elements of amino acids, is vital to living organisms. The accelerating exploitation of nitrogen‐containing compounds has brought global environmental contamination and an energy crisis . In particular, ammonia (NH 3 ) is one of the most common industrial chemicals.…”

Section: Figurementioning

confidence: 99%

“…The accelerating exploitation of nitrogencontaining compounds has brought global environmental contamination and an energy crisis. [1,2] In particular, ammonia (NH 3 ) is one of the most common industrial chemicals. It not only plays a significant role in agriculture, textile industries, plastics, and the pharmaceutical industry, [3][4][5] but also shows promise as a next-generation energy carrier owing to its high energy density (4.3 kWh kg À1 ) and clean emissions.…”

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confidence: 99%

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Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

et al. 2020

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Unveiling the active phase of catalytic materials under reaction conditions is important for the construction of efficient electrocatalysts for selective nitrate reduction to ammonia. The origin of the prominent activity enhancement for CuO (Faradaic efficiency: 95.8 %, Selectivity: 81.2 %) toward selective nitrate electroreduction to ammonia was probed. 15N isotope labeling experiments showed that ammonia originated from nitrate reduction. 1H NMR spectroscopy and colorimetric methods were performed to quantify ammonia. In situ Raman and ex situ experiments revealed that CuO was electrochemically converted into Cu/Cu2O, which serves as an active phase. The combined results of online differential electrochemical mass spectrometry (DEMS) and DFT calculations demonstrated that the electron transfer from Cu2O to Cu at the interface could facilitate the formation of *NOH intermediate and suppress the hydrogen evolution reaction, leading to high selectivity and Faradaic efficiency.

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Section: Figurementioning

confidence: 99%

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confidence: 99%

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

et al. 2020

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“…[5] Nevertheless, this process is still in its infancy stage, thus rigorous and reliable protocols to evaluate the activity of the catalysts are necessary and highly concerned. [6][7][8] Also, recent reports have mentioned that the employed Nafion 2 µg mL −1 of ammonia-containing electrolyte for an example, this will lead to a measurement error of ≈30 wt%. Moreover, it was worth noting that the ammonia transferred from cathode cell may be electrooxidized at the anode owing to the high potential of the anode, and this possibility was investigated and revealed in a typical single cell schemed in Figure S7 of the Supporting Information.…”

Section: Electrocatalytic N 2 Reductionmentioning

confidence: 99%

Is It Appropriate to Use the Nafion Membrane in Electrocatalytic N₂ Reduction?

Ren

Tan

et al. 2019

Small Methods

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The electrocatalytic N2 reduction reaction (ENRR) to ammonia has attracted much attention due to the mild operating conditions, in which the Nafion membrane is generally adopted to separate the ammonia from the anode products. However, it has been mentioned that the Nafion membrane allows ammonia to pass through and traps the ammonia to some extent, but powerful confirmation experiments and effective solutions are still lacking. Herein, it is experimentally confirmed that the use of the Nafion membrane in the ENRR is inappropriate, based on the results that the ammonia can pass through the membrane, be adsorbed on the membrane, and interact with the membrane. This causes a measurement error and accelerates the membrane degradation process, which is unfavorable for ammonia quantification and the long‐term stability operation of the ENRR in practical application. Also, for the first time, a more accurate method to evaluate the activity of the ENRR electrocatalyst using a salt bridge to replace the Nafion membrane is presented.

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“…Therefore, nitrides can be said to exhibit NRR performance only when the NH 3 production rate is larger than or equal to their decomposition rate. Additionally, some control experiments can also be undertaken to determine the origin of NH 3 , according to the procedure proposed recently . During NRR, both the anion in the metal compounds and the cation (Mn) can escape, leading to a defective, oxygen‐abundant surface structure of Mn 3 O 4 for more favorable NRR …”

Section: Design Principles For Electrocatalystsmentioning

confidence: 99%

“…Additionally, some control experiments can also be undertaken to determine the origin of NH 3 , according to the procedure proposed recently. [114][115][116] During NRR, both the anion in the metal compounds and the cation (Mn) can escape, leading to a defective, oxygen-abundant surface structure of Mn 3 O 4 for more favorable NRR. [117] Beyond in situ vacancy generation during NRR, defects can also be created during synthesis of many metal materials.…”

Section: Defective Metal Materialsmentioning

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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How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully

Abstract: A guidebook with best practices and potential opportunities to explore ambient electrocatalytic nitrogen reduction reliably and insightfully.

Cited by 804 publications

References 48 publications

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Is It Appropriate to Use the Nafion Membrane in Electrocatalytic N₂ Reduction?

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

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How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully

Abstract: A guidebook with best practices and potential opportunities to explore ambient electrocatalytic nitrogen reduction reliably and insightfully.

Cited by 804 publications

References 48 publications

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Is It Appropriate to Use the Nafion Membrane in Electrocatalytic N2 Reduction?

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

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Is It Appropriate to Use the Nafion Membrane in Electrocatalytic N₂ Reduction?