Efficient electrocatalytic nitric oxide reduction to ammonia using manganese spinel oxides

Niu, Zhaodong; Fan, Shiying; Li, Xinyong

doi:10.1039/d4ta03153a

J. Mater. Chem. A

2024

DOI: 10.1039/d4ta03153a

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Efficient electrocatalytic nitric oxide reduction to ammonia using manganese spinel oxides

Zhaodong Niu,

Shiying Fan,

Xinyong Li

Abstract: Electrocatalytic nitric oxide (NO) reduction reaction (NORR) driven by renewable electricity is a sustainable route for air pollution treatment and ammonia (NH3) synthesis. Herein, we report a carbon fiber-supported CoMn2O4...

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Cited by 2 publications

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Electrode Materials for NO Electroreduction Based on Dithiolene Metal–Organic Frameworks: A Theoretical Study

Fan,

Yang,

et al. 2024

Catalysts

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To quickly and efficiently screen catalytic materials with both activity and selectivity for the nitric oxide reduction reaction (NORR), we adopted a strategy that considers the activity of the side reaction hydrogen evolution reaction (HER) first. It can be seen that Fe3(THT)2 (THT = triphenylene-2,3,6,7,10,11-hexathiol) has extremely excellent HER activity, with a Gibbs free energy change (ΔG) of 0.007 eV. Based on the relationship between ΔG and theoretical exchange current density, all TM3(THT)2 can be divided into two regions: one is the absolute values of ΔG greater than 1 eV, the other is the absolute values of ΔG greater than 0 eV and less than 1eV. Obviously, the candidates with the absolute values of ΔG greater than 1 eV have poor HER performance, but this precisely provides the possibility of obtaining NORR catalytic materials with both excellent selectivity and activity. Subsequent calculation results show that the maximum ΔG change of the rate-determining step of Ta3(THT)2 is unexpectedly only 0.05 eV. Therefore, Ta3(THT)2 may be regarded as the NORR catalytic material with both excellent performance and selectivity. Based on the electron transfer and partial density of states (PDOS) analysis, it can be seen that Ta plays a crucial role in the activation stage of NO. The approach that considers the activity of the side reaction HER first may provide a new idea for rapidly screening highly selective and active NORR catalysts.

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Electrode Materials for NO Electroreduction Based on Dithiolene Metal–Organic Frameworks: A Theoretical Study

Fan,

Yang,

et al. 2024

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Electrochemical Ammonia Synthesis from Dilute Gaseous Nitric Oxide Reduction at Ambient Conditions

Rasheed,

Kim,

Kim

et al. 2024

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Converting gaseous nitric oxide (NO) to ammonia (NH3) is important because of its environmental and industrial implications. The electrochemical transformation of nitrogen (N2) to NH3 faces several challenges, including a slow reaction rate and low Faradaic efficiency (FE). This study presents an innovative approach by integrating NO elimination and NH3 production by electrochemical gaseous NO reduction reaction (NORR) under ambient conditions. Co and Mo-based catalysts were investigated for the continuous reduction of diluted NO gas (1%) to NH3 within a proton exchange membrane (PEM) cell under ambient conditions. In electrochemical NORR tests conducted without a catholyte, CoMo-NC demonstrated notable NORR performance, achieving an NH3 yield rate of 23.2 × 10−10 mol s−1 cm−2 at −2.2 Vcell and FENH3 of 94.6% at −1.6 Vcell, along with enhanced durability. Notably, this performance represents one of the highest FENH3 achievements for electrochemical gas-phase NO reduction at room temperature.

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Efficient electrocatalytic nitric oxide reduction to ammonia using manganese spinel oxides

Abstract: Electrocatalytic nitric oxide (NO) reduction reaction (NORR) driven by renewable electricity is a sustainable route for air pollution treatment and ammonia (NH3) synthesis. Herein, we report a carbon fiber-supported CoMn2O4...

Cited by 2 publications

References 52 publications

Electrode Materials for NO Electroreduction Based on Dithiolene Metal–Organic Frameworks: A Theoretical Study

Electrode Materials for NO Electroreduction Based on Dithiolene Metal–Organic Frameworks: A Theoretical Study

Electrochemical Ammonia Synthesis from Dilute Gaseous Nitric Oxide Reduction at Ambient Conditions

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