Issue 12, 2024

Cold plasma activated Ni0/Ni2+ interface catalysts for efficient electrocatalytic methane oxidation to low-carbon alcohols

Abstract

The field of converting methane into valuable products using renewable energy sources under ambient conditions is both appealing and highly demanding. The inherent inertness of methane (CH4) necessitates the selective breaking of its first C–H bond while avoiding excessive oxidation, in order to transform CH4 into high-value products. Herein we present a novel approach for creating a highly concentrated Ni0/Ni2+-on-Cu interface using an O2 cold plasma in situ method to enhance the activity and stability of the CH4OR to low-carbon alcohol. The Cu@Ni–NiO electrocatalyst exhibits excellent performance for the CH4OR to low-carbon alcohol, showcasing a high faradaic efficiency (FE) of 86.7%, an impressive low-carbon alcohol yield of 1215.2 μmol g−1 h−1, remarkable durability (66 h) and a notable C2H5OH selectivity of 59.8% at 1.9 V vs. RHE. The ATRSEIRAS spectroscopy and DFT calculations further reveal that the synergistic effect of the Ni0/Ni2+-on-Cu interface can enhance the *O and *CH2 generation on Ni0, and the *CH2 spillover from Ni0 to Ni2+ atoms can also improve the C–C coupling reaction. Additionally, the in situ treatment with O2 cold plasma can enhance the formation of NiO, leading to a high concentration of the Ni0/Ni2+-on-Cu interface, which effectively prevents the oxidation of Ni0 during the CH4OR process. Furthermore, we developed a general oxidation strategy for the direct synthesis of transition metal nitrides by O2 cold plasma treatment of Ni0. Compared with the previous methods used for the preparation of NiO, the Ni-based metal oxide synthesis method offers several advantages, including simplicity and practicality, low cost, high throughput, pollution-free nature, low energy consumption and the capability to prepare metal oxides with controllable coordination number of the O atom. This work provides new insights into the highly efficient CH4OR process and presents an innovative, cost-effective method for preparing electrocatalysts.

Graphical abstract: Cold plasma activated Ni0/Ni2+ interface catalysts for efficient electrocatalytic methane oxidation to low-carbon alcohols

Supplementary files

Article information

Article type
Paper
Submitted
18 Jan 2024
Accepted
07 May 2024
First published
15 May 2024

Green Chem., 2024,26, 7091-7100

Cold plasma activated Ni0/Ni2+ interface catalysts for efficient electrocatalytic methane oxidation to low-carbon alcohols

Q. Zhang, W. Li, J. Peng, L. Xue and G. He, Green Chem., 2024, 26, 7091 DOI: 10.1039/D4GC00289J

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