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

Wang, Yuting; Zhou, Wei; Jia, Ranran; Yu, Yifu; Zhang, Bin

doi:10.1002/anie.201915992

Cited by 1,072 publications

(918 citation statements)

References 49 publications

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“…[30] Twofold coordination is sterically favorable for the cleavage of the NO bond and had been employed in the first principles calculation for the mechanism of electrochemical reduction on catalysts. [30][31][32]…”

Section: Kinetic Mechanisms Of Electrochemical Nitrate Reductionmentioning

confidence: 99%

Restoring the Nitrogen Cycle by Electrochemical Reduction of Nitrate: Progress and Prospects

et al. 2020

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The increasing amount of anthropogenic nitrogen has resulted in alarming levels of nitrate in bodies of water and caused a cascade of damage to the environment and human health. Electrochemical nitrate reduction is an efficient strategy ancillary to biological nitrogen cycle management, which utilizes electrons as green reductants and rebalances the N 2 cycle. In this review, the fundamental principles and implementation of electrochemical nitrate reduction are described to lay the foundation for the eventual large-scale application in the remediation of nitrate-laden wastewaters. Factors that influence the activity and selectivity of electrochemical nitrate reduction are also discussed. Moreover, electrolytic cell design and construction are discussed via a rational choice of critical components and assembly. Finally, a roadmap for the development of highly selective nitrate reduction catalysts is proposed. This review attempts to provide a practical strategy for electrochemical nitrogen cycle management and aims to stimulate future research for final implementation.

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Section: Kinetic Mechanisms Of Electrochemical Nitrate Reductionmentioning

confidence: 99%

Restoring the Nitrogen Cycle by Electrochemical Reduction of Nitrate: Progress and Prospects

et al. 2020

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“…From the perspective of environmental scientists, the most desirable solution for nitrate removal is to selectively reduce it to harmless gaseous nitrogen, but few non‐noble metal catalysts available today can convert nitrate into nitrogen with a high selectivity. In this regard, recent studies [ 13–16 ] by chemical scientists have attempted to promote the selectively electrocatalytic reduction of nitrate to ammonia, a value‐added product utilized as a precursor to fertilizer.…”

Section: Introductionmentioning

confidence: 99%

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

Zhu

Chen

Liao

et al. 2020

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Metallic Cu is a well-known electrocatalyst for nitrate reduction reaction (NO 3 RR), but it suffers from relatively low activity, poor stability, and inducing nitrite accumulation during the long-term operation. Herein, it is found that Cu catalysts minimized at the single-atom level can overcome the limitations of bulk materials in NO 3 RR. A metal-nitrogen-carbon (M-N-C) electrocatalyst composed of carbon nanosheets embedding isolated copper atoms coordinated with N, Cu-N-C-800, is synthesized by pyrolysis of a Cu-based metal-organic framework at 800 °C. In comparison with Cu nanoparticles and Cu plate-800, kinetic measurements show that the Cu-N-C-800 electrocatalyst is more active and stable and distinctly suppresses the release of nitrite intermediate into the solution. The combined results of experimental data and density functional theory calculations indicate that Cu bound with N (particularly Cu-N 2) is the key to favorable adsorption of NO 3 − and NO 2 −. This strong binding is responsible for the enhanced rate of nitrate conversion to the end products of ammonia and nitrogen. These findings highlight the promise of single-atom Cu electrocatalysts for nitrate reduction with desirable performance.

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“…Thus, the elaborate design and construction of efficient electrocatalysts is critical. Recently, we reported that the selectivity and Faradaic efficiency of Cu for electrocatalytic NO 3 − reduction to ammonia could be enhanced by the modification of its electronic structure [28]. Moreover, constructing Schottky junctions has been proved as an efficient strategy to modulate the electron density at the interface of the Schottky electrocatalysts [29,30].…”

Section: Introductionmentioning

confidence: 99%

Promoting selective electroreduction of nitrates to ammonia over electron-deficient Co modulated by rectifying Schottky contacts

et al. 2020

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Developing efficient electrocatalysts for selective nitrate contamination reduction into value-added ammonia is significant. Here, heterostructured Co/CoO nanosheet arrays (Co/CoO NSAs) exhibited excellent Faradaic efficiency (93.8%) and selectivity (91.2%) for nitrate electroreduction to ammonia, greatly outperforming Co NSAs. 15 N isotope labeling experiments and 1 H nuclear magnetic resonance (NMR) quantitative testing methods confirmed the origin of the produced ammonia. Electrochemical in situ Fourier transform infrared (FTIR) spectroscopy, online differential electrochemical mass spectrometry (DEMS) data and density functional theory (DFT) results revealed that the superior performances arose from the electron deficiency of Co induced by the rectifying Schottky contact in the Co/CoO heterostructures. The electron transfer from Co to CoO at the interface could not only suppress the competitive hydrogen evolution reaction, but also increase energy barriers for by-products, thus leading to high Faradaic efficiency and selectivity of ammonia.

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

Cited by 1,072 publications

References 49 publications

Restoring the Nitrogen Cycle by Electrochemical Reduction of Nitrate: Progress and Prospects

Restoring the Nitrogen Cycle by Electrochemical Reduction of Nitrate: Progress and Prospects

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

Promoting selective electroreduction of nitrates to ammonia over electron-deficient Co modulated by rectifying Schottky contacts

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