Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation

甲醇 催化作用 石墨烯 材料科学 异质结 纳米片 贵金属 纳米颗粒 直接甲醇燃料电池 化学工程 甲醇燃料 阳极 金属 纳米技术 化学 电极 物理化学 光电子学 工程类 有机化学 冶金 生物化学
作者
Qi Zhang,Quanguo Jiang,Xiang Yang,Chi Zhang,Jian Zhang,Lu Yang,Haiyan He,Guobing Ying,Huajie Huang
出处
期刊:Journal of Energy Chemistry [Elsevier BV]
卷期号:93: 419-428 被引量:53
标识
DOI:10.1016/j.jechem.2024.02.038
摘要

Although metallic rhodium (Rh) is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell (DMFC), the conventional "particle-to-face" contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects. Herein, we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti3C2Tx MXene nanolamellas (Rh NS/MXene) via a convenient stereoassembly process. This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features, including large accessible surface areas, strong "face-to-face" interfacial interactions, homogeneous Rh nanosheet distribution, ameliorative electronic structure, and high electronic conductivity. As a consequence, the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m2 g−1Rh, a high mass activity of 1056.9 mA mg−1Rh, and a long service life, which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black, carbon nanotubes, reduced graphene oxide, and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount. Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center, thereby making the Rh NS/MXene configuration suffer less from CO poisoning. This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts, which may provide new avenues for developing the next-generation DMFC devices.
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