期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 2, 页码 2400-2406出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b17088
关键词
MXene termination; palladium catalyst; electrocatalysis; surface chemistry; strong metal-support interaction
资金
- National Natural Science Foundation of China [51872218, 21673171]
- Fundamental Research Funds for the Central Universities [2019-zy-041]
- State Key Laboratory of Advanced Technology for Materials Sythesis and Processing [WUT: 2019-KF-2, 2019-KF-5]
- UK National Measurement System
Efficient catalysis of the methanol oxidation reaction (MOR) greatly determines the widespread implementation of direct methanol fuel cells. Exploring a suitable support for noble metal catalysts with regard to decreasing the mass loading and optimizing the MOR activity remains a key challenge. Herein, we achieve an over 60% activity enhancement of a palladium (Pd) catalyst by introducing a two-dimensional Ti3C2Tx MXene as the support compared to a commercial Pd/C catalyst. Not only are more catalytically active Pd sites exposed on the Pd/MXene catalyst while maintaining a low mass loading, but the introduction of the MXene support also significantly alters the surface electronic structure of Pd. Specifically, spectroscopy and density functional theory (DFT) computations indicate that sufficiently electronegative terminations of the Ti3C2Tx MXene surface can induce strong metal-support interactions (SMSI) with the Pd catalyst, leading to optimal methanol adsorption. This MXene-supported Pd catalyst exhibits a much higher MOR current density (12.4 mA cm(-2)) than that of commercial Pd/C (7.6 mA cm(-2)). Our work largely optimizes the intrinsic activity of a Pd catalyst by the utilization of MXene surface terminations, and the crucial SMSI effects revealed herein open a rational avenue to the design of more efficient noble metal catalysts for MOR.
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