Electrochemical reduction of NOx species at the interface of nanostructured Pd and PdCu catalysts in alkaline conditions

Soto-Hernández, J.; Santiago-Ramírez, C. R.; Ramírez-Meneses, E.; Luna-Trujillo, Mayra; Wang, Jinan; Lartundo-Rojas, L.; Manzo-Robledo, A.

doi:10.1016/j.apcatb.2019.118048

Cited by 70 publications

(47 citation statements)

References 45 publications

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“…The MS probe was placed near the working electrode from the gas channel side, and the MS signals linked to possible products were tracked over time. We conducted the FEMS measurement on the Cu catalyst using 0.83% NO in Ar (in the absence of CO 2 ), because the ionization of N 2 (m/z = 28,14) and N 2 O (m/z = 44, 30,28,14) produces the same fragments with CO 2 and various CO 2 reduction products [31][32][33] , complicating the reliable analysis of the NORR products (see Supplementary Note for more details). MS signals of the FEMS measurement under a continuous feed of 0.83% NO are presented in Fig.…”

Section: Resultsmentioning

confidence: 99%

“…The electrochemical reduction products of NO, the major component of NO x in industrial point sources, were further investigated. As NH 3 , NH 2 OH, N 2 , and N 2 O have been suggested as the main products in NORR 26 , 28 , 29 , NH 3 and NH 2 OH were detected via spectrophotometry (Supplementary Figs. 13 and 14 ), and N 2 was detected via GC (Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

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The impact of nitrogen oxides on electrochemical carbon dioxide reduction

et al. 2020

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The electroreduction of carbon dioxide offers a promising avenue to produce valuable fuels and chemicals using greenhouse gas carbon dioxide as the carbon feedstock. Because industrial carbon dioxide point sources often contain numerous contaminants, such as nitrogen oxides, understanding the potential impact of contaminants on carbon dioxide electrolysis is crucial for practical applications. Herein, we investigate the impact of various nitrogen oxides, including nitric oxide, nitrogen dioxide, and nitrous oxide, on carbon dioxide electroreduction on three model electrocatalysts (i.e., copper, silver, and tin). We demonstrate that the presence of nitrogen oxides (up to 0.83%) in the carbon dioxide feed leads to a considerable Faradaic efficiency loss in carbon dioxide electroreduction, which is caused by the preferential electroreduction of nitrogen oxides over carbon dioxide. The primary products of nitrogen oxides electroreduction include nitrous oxide, nitrogen, hydroxylamine, and ammonia. Despite the loss in Faradaic efficiency, the electrocatalysts exhibit similar carbon dioxide reduction performances once a pure carbon dioxide feed is restored, indicating a negligible long-term impact of nitrogen oxides on the catalytic properties of the model catalysts.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

The impact of nitrogen oxides on electrochemical carbon dioxide reduction

et al. 2020

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“…More importantly, electrodes, electrocatalysts, electrolytes, solvents and any other component of the experimental setup that is nitrogenbased or was prepared using N-containing precursor(s) can be a source of contamination. In this scenario, ammonia can be either released spontaneously upon bringing different components into [27][28][29][30][54][55][56][57] of some of the known electrocatalysts for each process.…”

Section: Potential Origins Of False Nrr Positivesmentioning

confidence: 99%

“…In particular, some papers, including those published in high-profile journals, discuss the feasibility of charge-transfer steps only, the thermodynamics of which can be favourably adjusted by "applying" an increasingly (sometimes unrealistic) negative potential, but ignore the very significant energy barriers, of the order of a few eV, for other steps such as N 2 adsorption or NH 3 desorption, which do not depend on the potential. For example, theoretical data of this kind appear in publications 3,23,29,40,41,51,55,82,92,97,105,109,112,116,122, and 123 in Supplementary Table 1. Significant disagreement between the theoretically predicted potentials required for the NRR with those reported experimentally is also not uncommon.…”

Section: Understanding Nrr Through Computational Chemistrymentioning

confidence: 99%

Identification and elimination of false positives in electrochemical nitrogen reduction studies

et al. 2020

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Ammonia is of emerging interest as a liquefied, renewable-energy-sourced energy carrier for global use in the future. Electrochemical reduction of N2 (NRR) is widely recognised as an alternative to the traditional Haber–Bosch production process for ammonia. However, though the challenges of NRR experiments have become better understood, the reported rates are often too low to be convincing that reduction of the highly unreactive N2 molecule has actually been achieved. This perspective critically reassesses a wide range of the NRR reports, describes experimental case studies of potential origins of false-positives, and presents an updated, simplified experimental protocol dealing with the recently emerging issues.

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“…NO x has been considered one of the major air pollutants, which do not only harm the human body, but also trigger a series of serious environmental problems like global warming, photochemical smog, ozone depletion, and respiratory diseases [3, 4, 5]. NOx further reacts with OH − radicals in the atmosphere to form nitric acid, thereby producing acid rain [6]. In addition, NOx causes the eutrophication of lakes, which brings to extinction of aquatic life [7].…”

Section: Introductionmentioning

confidence: 99%

Nitrogen oxide reduction through absorbent solutions containing nitric acid and hydrogen peroxide in hollow fiber membrane modules

Kartohardjono

Merry

Rizky

et al. 2019

Heliyon

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Emissions of nitrogen oxides such as NO and NO2, which are commonly known as NOx, are threats to human existence and cause environmental problems. Mainly, two techniques have been developed to drastically reduce these emissions, which are dry and wet processes. The wet process has several advantages, major identifiable advantages are the adaptability to the flue gas, low operating temperatures and no poisoning and inactivation catalyst. Also, a mixture of hydrogen peroxide and nitric acid are used as absorbents solution for NOx reduction in the wet process. The advantages of using this mixture include the ability to reduce the negative effect of NOx and does not contaminate the scrubbing solution. In addition, nitric acid has an economical advantage in the process considering the fact that it is produced in the process. Finally, it can be conducted at ambient temperature. This study furthermore used a mixture of hydrogen peroxide and nitric acid solutions as an absorbent to reduce NOx in hollow fiber membrane modules. The hydrogen peroxide oxidized HNO2 to nitric acid, while enhances the oxidation through an autocatalytic reaction. The effects of the feed gas flow rate, hydrogen peroxide concentrations and number of fibers on the NOx reduction, absorbed NOx and flux were varied to study. The experimental results showed that the increase in the feed gas flow rate from 100 to 200 mL/min decreased NOx reduction from about 98 to 94% but increased the absorbed NOx and flux from about 0.13 to 0.255 mmol/h and 0.85–1.63 mmol/m2.h, respectively The increase in proportion of NOx in the feed gas effect was dominant than the increase in absorbed NOx. An increase in hydrogen peroxide concentration from 0.5 to 10 wt.% in the absorbent solutions increased NOx reduction, absorbed NOx and flux from about 94 to 98%, 0.257–0.267 mmol/h and 1.09–1.13 mmol/m2.h, respectively. Additionally, the H2O2 plays an important role in enhancing HNO2 oxidation to HNO3. Furthermore, an increase in the number of fibers from 50 to 150 in the membrane module increased NOx reduction and absorbed NOx from 86 to 97% and 0.23–0.27 mmol/h. Flux decreased from 2.98 to 1.13 mmol/m2.h due to increment in the gas-liquid contact surface area.

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Electrochemical reduction of NOx species at the interface of nanostructured Pd and PdCu catalysts in alkaline conditions

Cited by 70 publications

References 45 publications

The impact of nitrogen oxides on electrochemical carbon dioxide reduction

The impact of nitrogen oxides on electrochemical carbon dioxide reduction

Identification and elimination of false positives in electrochemical nitrogen reduction studies

Nitrogen oxide reduction through absorbent solutions containing nitric acid and hydrogen peroxide in hollow fiber membrane modules

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