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Free radicals promote electrocatalytic nitrogen oxidation.

ABSTRACT: In this work, we introduce hydroxyl radicals into the electrocatalytic nitrogen oxidation reaction (NOR) for the first time. Cobalt tetroxide (Co₃O₄) acts not only as an electrocatalyst, but also as a nanozyme (in combination with hydrogen peroxide producing ˙OH), and can be used as a high-efficiency nitrogen oxidation reaction (NOR) electrocatalyst for environmental nitrate synthesis. Co₃O₄ + ˙OH shows an excellent nitrogen oxidation reaction (NOR) performance among Co₃O₄ catalysts in 0.1 M Na₂SO₄ solution. At an applied potential of 1.7 V vs. RHE, the HNO₃ yield of Co₃O₄ + ˙OH reaches 89.35 μg h^-1 mg_cat ^-1, which is up to 7 times higher than that of Co₃O₄ (12.8 μg h^-1 mg_cat ^-1) and the corresponding FE is 20.4%. The TOF of Co₃O₄ + ˙OH at 1.7 V vs. RHE reaches 0.58 h^-1, which is higher than that of Co₃O₄ (0.083 h^-1), demonstrating that free radicals greatly enhance the intrinsic activity. Density functional theory (DFT) demonstrates that ˙OH not only can drive nitrogen adsorption, but also can decrease the energy barrier (rate-determining step) of N₂ to N₂OH*, thus producing great NOR activity.

SUBMITTER: Wang Z

PROVIDER: S-EPMC9930917 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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Free radicals promote electrocatalytic nitrogen oxidation.

Wang Zuochao Z Liu Jiao J Zhao Huan H Xu Wenxia W Liu Jiaxin J Liu Ziyi Z Lai Jianping J Wang Lei L

Chemical science 20230126 7

In this work, we introduce hydroxyl radicals into the electrocatalytic nitrogen oxidation reaction (NOR) for the first time. Cobalt tetroxide (Co3O4) acts not only as an electrocatalyst, but also as a nanozyme (in combination with hydrogen peroxide producing ˙OH), and can be used as a high-efficiency nitrogen oxidation reaction (NOR) electrocatalyst for environmental nitrate synthesis. Co3O4 + ˙OH shows an excellent nitrogen oxidation reaction (NOR) pe ...[more]

PMID: 36819849

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Project description:Simple Summary It is vitally important that scientists are able to describe their work simply and concisely to the public, especially in an open access online journal. The simple summary consists of no more than 200 words in one paragraph and contains a clear statement of the problem addressed, the aims and objectives, pertinent results, conclusions from the study, and how they will be valuable to society. This should be written for a lay audience, i.e., no technical terms without explanations. No references are cited, and no abbreviations included. Submissions without a simple summary will be returned directly. Abstract Developing renewable energy sources and controlling water pollution are critical but challenging problems. Urea oxidation (UOR) and methanol oxidation (MOR), both of which have high research value, have the potential to effectively address wastewater pollution and energy crisis problems. A three-dimensional neodymium-dioxide/nickel-selenide-modified nitrogen-doped carbon nanosheet (Nd2O3-NiSe-NC) catalyst is prepared in this study by using mixed freeze-drying, salt-template-assisted technology, and high-temperature pyrolysis. The Nd2O3-NiSe-NC electrode showed good catalytic activity for MOR (peak current density ~145.04 mA cm−2 and low oxidation potential ~1.33 V) and UOR (peak current density ~100.68 mA cm−2 and low oxidation potential ~1.32 V); the catalyst has excellent MOR and UOR characteristics. The electrochemical reaction activity and the electron transfer rate increased because of selenide and carbon doping. Moreover, the synergistic action of neodymium oxide doping, nickel selenide, and the oxygen vacancy generated at the interface can adjust the electronic structure. The doping of rare-earth-metal oxides can also effectively adjust the electronic density of nickel selenide, allowing it to act as a cocatalyst, thus improving the catalytic activity in the UOR and MOR processes. The optimal UOR and MOR properties are achieved by adjusting the catalyst ratio and carbonization temperature. This experiment presents a straightforward synthetic method for creating a new rare-earth-based composite catalyst.

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Free radicals promote electrocatalytic nitrogen oxidation.

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Free radicals promote electrocatalytic nitrogen oxidation.

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