Synergistic Cu@CoOx core-cage structure on carbon layers as highly active and durable electrocatalysts for methanol oxidation----Beijing Synchrotron Radiation Facility

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Synergistic Cu@CoOx core-cage structure on carbon layers as highly active and durable electrocatalysts for methanol oxidation

From：　 PublishDate：2020-07-30　 Hits：

Active and inexpensive electrocatalysts for methanol oxidation reaction (MOR) are highly required for the practical application of direct methanol fuel cells (DMFCs). However, efficient MOR is limited by using the expensive and rare noble metal-based catalysts. A team from the Institute of Functional Nano & Soft Materials Laboratory in Soochow university reported a Cu@CoOx core-cage nanostructure on carbon layers (CLs) for superior electrocatalysis of MOR in the alkaline media. The related research result was published in "Applied Catalysis B: Environmental" on May 5, 2019.

They found that Cu@CoOx-CLs was an excellent catalyst for methanol oxidation. It showed an excellent specific activity of 150.41 mA cm^-2 and a high mass activity of 467.94 mA mg^-1 at the potential of 0.8 V vs. SCE in 1M KOH+1M CH₃OH, which was one of the best methanol oxidation performance ever reported for noble metal-free catalysts. It also showed an impressive long-term durability (≥ 10,800 s). Adsorption experiments indicated that Cu could act as the methanol adsorption center. In-situ XAS experiments revealed that the CoOx cage with a high intermediate Co4+ state in MOR could effectively accelerate the reaction while Cu remained a low chemical state.

The in-situ XAS experiment was performed at BSRF (1W1B). The XAS results revealed that the valence state of Co changed with the applied external voltage. Specifically, when the voltage reached 0.83 V vs. SCE, a higher Co⁴⁺ intermediate state could be observed to effectively oxidize methanol and then accelerate the MOR process. Moreover, When the reaction finished (back to 0 V vs. SCE), the spectrum could recover to the initial state (similar energy position), confirming the reversible Co state as a good catalyst. Cu showed a stable low chemical state during the reaction.

Article:

Yue Sun¹, Yunjie Zhou¹, Cheng Zhu, Wenjing Tu, Huibo Wang, Hui Huang, Yang Liu*, Mingwang Shao*, Jun Zhong*, Shuit-Tong Lee, Zhenhui Kang*, Synergistic Cu@CoOx core-cage structure on carbon layers as highly active and durable electrocatalysts for methanol oxidation. Applied Catalysis B: Environmental 2019, 244, 795-801.

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