Issue 16, 2024

Efficient electrochemical coupling of nitrate and biomass-derived acetone to acetoxime at a high current density over a Zn/Cu hexagonal nanosheet catalyst

Abstract

Acetoxime, as an important type of organic compound containing a C[double bond, length as m-dash]N bond, is commonly employed as a boiler chemical deoxygenation agent and boiler acid pickling passivator due to its low toxicity and high reducibility characteristics. The conventional synthesis of acetoxime involves the initial catalysis of NOx and H2 under harsh conditions by noble metal catalysts to generate unstable NH2OH, which further reacts with acetone to form acetoxime. Herein, we report a Zn/Cu/CF hexagonal ultrathin nanosheet catalyst capable of efficiently catalyzing the coupling reaction between NH2OH produced in situ from electrocatalytic NO3 reduction and CH3COCH3 to generate an oxime under ambient conditions. The presence of Cu facilitates the conversion of NO3, while the introduction of Zn is favourable to accelerate the electron transfer rate, enhance the number of active sites, and suppress the reduction hydrogenation of *CH3COCH3, thereby significantly improving the activity of oxime. Through catalyst screening and the optimization of electrolysis conditions, a faradaic efficiency of 44.5% with a yield rate of 415.5 μmol cm−2 h−1 is achieved at an industrially relevant current density of −150 mA cm−2 in the electrolyte containing 0.2 M NO3 + 0.2 M CH3COCH3 over the Zn/Cu-CF-6 electrocatalyst, corresponding to a C selectivity approaching 100%. A series of control experiments and in situ characterization studies indicate that *NH2OH and *CH3COCH3 are crucial intermediates for the synthesis of acetoxime, proposing a plausible reaction pathway. This work presents a facile synthesis method for Zn/Cu/CF hexagonal nanosheet catalysts and proposes a green strategy for the one-pot efficient electrochemical synthesis of acetoxime from pollutants NO3 and biomass-derived acetone, offering a green pathway for high-value-added C[double bond, length as m-dash]N product synthesis.

Graphical abstract: Efficient electrochemical coupling of nitrate and biomass-derived acetone to acetoxime at a high current density over a Zn/Cu hexagonal nanosheet catalyst

Supplementary files

Article information

Article type
Research Article
Submitted
16 Mai 2024
Accepted
19 Jun 2024
First published
20 Jun 2024

Inorg. Chem. Front., 2024,11, 5286-5298

Efficient electrochemical coupling of nitrate and biomass-derived acetone to acetoxime at a high current density over a Zn/Cu hexagonal nanosheet catalyst

J. Shao, Y. Zhang, S. Xue, Z. Li, X. Li, B. Liang, T. Li, H. Dong and Y. Zhang, Inorg. Chem. Front., 2024, 11, 5286 DOI: 10.1039/D4QI01234H

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