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Cold plasma activated Ni0/Ni2+ interface catalysts for efficient electrocatalytic methane oxidation to low-carbon alcohols.
- Source :
- Green Chemistry; 6/21/2024, Vol. 26 Issue 12, p7091-7100, 10p
- Publication Year :
- 2024
-
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 (CH<subscript>4</subscript>) necessitates the selective breaking of its first C–H bond while avoiding excessive oxidation, in order to transform CH<subscript>4</subscript> into high-value products. Herein we present a novel approach for creating a highly concentrated Ni<superscript>0</superscript>/Ni<superscript>2+</superscript>-on-Cu interface using an O<subscript>2</subscript> cold plasma in situ method to enhance the activity and stability of the CH<subscript>4</subscript>OR to low-carbon alcohol. The Cu@Ni–NiO electrocatalyst exhibits excellent performance for the CH<subscript>4</subscript>OR to low-carbon alcohol, showcasing a high faradaic efficiency (FE) of 86.7%, an impressive low-carbon alcohol yield of 1215.2 μmol g<superscript>−1</superscript> h<superscript>−1</superscript>, remarkable durability (66 h) and a notable C<subscript>2</subscript>H<subscript>5</subscript>OH selectivity of 59.8% at 1.9 V vs. RHE. The ATRSEIRAS spectroscopy and DFT calculations further reveal that the synergistic effect of the Ni<superscript>0</superscript>/Ni<superscript>2+</superscript>-on-Cu interface can enhance the *O and *CH<subscript>2</subscript> generation on Ni<superscript>0</superscript>, and the *CH<subscript>2</subscript> spillover from Ni<superscript>0</superscript> to Ni<superscript>2+</superscript> atoms can also improve the C–C coupling reaction. Additionally, the in situ treatment with O<subscript>2</subscript> cold plasma can enhance the formation of NiO, leading to a high concentration of the Ni<superscript>0</superscript>/Ni<superscript>2+</superscript>-on-Cu interface, which effectively prevents the oxidation of Ni<superscript>0</superscript> during the CH<subscript>4</subscript>OR process. Furthermore, we developed a general oxidation strategy for the direct synthesis of transition metal nitrides by O<subscript>2</subscript> cold plasma treatment of Ni<superscript>0</superscript>. 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 CH<subscript>4</subscript>OR process and presents an innovative, cost-effective method for preparing electrocatalysts. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 14639262
- Volume :
- 26
- Issue :
- 12
- Database :
- Complementary Index
- Journal :
- Green Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 177927861
- Full Text :
- https://doi.org/10.1039/d4gc00289j