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Modification of the CuO electronic structure for enhanced selective electrochemical CO2 reduction to ethylene
Nano Research
Available online: 17 April 2024
Downloads:23

Electrochemical carbon dioxide reduction reaction (CO2RR) can produce value-added hydrocarbons from renewable electricity, providing a sustainable and promising approach to meet dual-carbon targets and alleviate the energy crisis. However, it is still challenging to improve the selectivity and stability of the products, especially the C2+ products. Here we propose to modulate the electronic structure of copper oxide (CuO) through lattice strain construction by zinc (Zn) doping to improve the selectivity of the catalyst to ethylene. Combined performance and in situ characterization analyses show that the compressive strain generated within the CuO lattice and the electronic structure modulation by Zn doping enhances the adsorption of the key intermediate *CO, thereby increasing the intrinsic activity of CO2RR and inhibiting the hydrogen precipitation reaction. Among the best catalysts had significantly improved ethylene selectivity of 60.5% and partial current density of 500 mA cm-2, and the highest C2+ Faraday efficiency of 71.47%. This paper provides a simple idea to study the modulation of CO2RR properties by heteroatom doped and lattice strain.

Research Article Issue
Mechanochemical route to fabricate an efficient nitrate reduction electrocatalyst
Nano Research 2024, 17 (6): 4889-4897
Published: 08 February 2024
Downloads:47

The electrochemical nitrate reduction reaction (NO3RR) to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies, but the progress of this reaction is impeded by the complex series of chemical reactions involving electron and proton transfer and competing hydrogen evolution reaction. Therefore, it becomes imperative to develop an electro-catalyst that exhibits exceptional efficiency and remarkable selectivity for ammonia synthesis while maintaining long-term stability. Herein the magnetic biochar (Fe-C) has been synthesized by a two-step mechanochemical route after a pyrolysis treatment (450, 700, and 1000 °C), which not only significantly decreases the particle size, but also exposes more oxygen-rich functional groups on the surface, promoting the adsorption of nitrate and water and accelerating electron transfer to convert it into ammonia. Results showed that the catalyst (Fe-C-700) has an impressive NH3 production rate of 3.5 mol·h−1·gcat−1, high Faradaic efficiency of 88%, and current density of 0.37 A·cm−2 at 0.8 V vs. reversible hydrogen electrode (RHE). In-situ Fourier transform infrared spectroscopy (FTIR) is used to investigate the reaction intermediate and to monitor the reaction. The oxygen functionalities on the catalyst surface activate nitrate ions to form various intermediates (NO2, NO, NH2OH, and NH2) and reduce the rate determining step energy barrier (*NO3 → *NO2). This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO3RR and opens the road for solving environmental and energy challenges.

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