The electrochemical reduction of nitrate over micro-architectured metal electrodes with stainless steel scaffold

Su, Jenn Fang; Ruzybayev, Inci; Shah, Ismat; Huang, C. P.

doi:10.1016/j.apcatb.2015.06.028

Cited by 133 publications

(64 citation statements)

References 47 publications

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“…24 ). The FE and yield rate of NO 3 – -to-NH 3 conversion on Fe SAC are orders of magnitude higher than reported N 2 -to-NH 3 conversions 10 , 21 , due to the dramatically different kinetic energy barriers to overcome 39 ; more importantly, the ammonia activity per metal active site favorably compare with other nitrate reduction systems which typically used bulk or nanostructured transition metal catalysts (Supplementary Table 3 ) 22 – 24 , 39 , 52 – 55 . Different from N 2 reduction studies where the concentrations of generated NH 3 are typically much lower than 1 H nuclear magnetic resonance (NMR) detection limit, in our case the generated NH 3 has concentrations high enough to be accurately quantified by NMR test, which helps to independently confirm our UV–Vis test.…”

Section: Resultsmentioning

confidence: 76%

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

et al. 2021

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Electrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h−1 mgcat.−1 (0.46 mmol h−1 cm−2). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites.

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Section: Resultsmentioning

confidence: 76%

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

et al. 2021

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“…The direct charge injection to NO 2 − leads to the formation of dianion radical NO 2 2− by Reaction (16). [ 52,53 ] Similar to the unstable NO 3 2− , the dianion radical NO 2 2− will quickly hydrolyze and produce NO (ad) (Reaction (17)) [ 54,55 ]

\begin{matrix} \begin{matrix} {NO}_{2 (ad)}^{-} + e^{-} \to {NO}_{2 (ad)}^{2 -} & E^{o} = - 0.47 V versus SHE \end{matrix} \end{matrix}

\begin{matrix} \begin{matrix} {NO}_{2 (ad)}^{2 -} + H_{2} O \to {NO}_{(ad)} + 2 {OH}^{-} & k = 1.0 \times 10^{5} s^{- 1} \end{matrix} \end{matrix}

…”

Section: Understanding Of Electrochemical Nitrate Reduction Mechanismsmentioning

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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“…Furthermore, several studies have investigated the nitrate electroreduction on different bimetallic, ternary metallic or alloy electrodes to improve the activity and the gaseous nitrogen selectivity due to the likely synergic effect between the different materials. For instance, significant improvement in the nitrate electroreduction was obtained with Cu-Ni [150][151][152][153], Cu-Sn [144], Cu-Rh [152,154], Cu-Zn [123,143,155] Cu-Pd [156][157][158][159], and Sn-Pd [160][161][162][163] cathodes, all of which have improved corrosion resistance and stability relative to monometallic Cu or Sn electrodes. In the case of the Cu-Zn cathode, ammonia was found as the main product by Mattarozzi et al [155].…”

Section: Electrode Materialsmentioning

confidence: 99%

“…On the other hand, although Pd cathodes have displayed practically no activity in nitrate electroreduction [159,160], they might enhance the electrocatalytic activity of Cu or Sn cathodes. In the case of Pd-Cu electrodes, the role of Cu is to promote the reduction of NO 3 to NO 2 -, and the role of Pd is to reduce nitrite to N 2 with high selectivity [156]. The use of higher amounts of Pd in the electrode composition has been shown to be beneficial towards N 2 selectivity.…”

Section: Electrode Materialsmentioning

confidence: 99%

State-of-the-art and perspectives of the catalytic and electrocatalytic reduction of aqueous nitrates

Martínez

Ortiz

Ortíz

2017

Applied Catalysis B: Environmental

425

280

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This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. State-of-the-art and perspectives of the catalytic and electrocatalytic reduction of aqueous nitrates.

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The electrochemical reduction of nitrate over micro-architectured metal electrodes with stainless steel scaffold

Cited by 133 publications

References 47 publications

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

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

State-of-the-art and perspectives of the catalytic and electrocatalytic reduction of aqueous nitrates

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