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Fabrication of 3D hollow acorn-shell-like PtBi intermetallics via a surfactant-free pathway for efficient ethylene glycol electrooxidation

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Nano Research 2023年第5期16卷 6560-6567页

作者： Tingting Wan Xin Huang Sichen Li Qiuyu Li Xianlong Yang Zhenjie Sun Dong Xiang Kun Wang Peng Li Manzhou Zhu Department of Chemistry and Center for Atomic Engineering of Advanced Materials School of Materials Science and EngineeringAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefei 230601China Key Laboratory of Structure and Functional Regulation of Hybrid Materials Ministry of EducationAnhui UniversityHefei 230601China

The synthesis of atomically ordered Pt-based intermetallic electrocatalysts for the direct alcohol fuel cells generally requires the addition of surfactants or the high-temperature annealing.However,some residual surfactants on the surface of the assynthesized catalysts would prevent the exposure of catalytic active sites,the high-temperature annealing process is easy to accelerate the sintering of the metal,which both lead to the decline of electrocatalytic performance.Herein,we construct the atomically ordered bimetallic PtBi intermetallics with clean surfaces and unique three-dimensional hollow acorn-shell-like structure(3D PtBi HASL)by a simple,low-temperature,surfactant-free one-pot synthetic approach.Benefiting from the special hollow structures,the obtained 3D PtBi HASL intermetallics expose abundant accessible active sites.Moreover,the introduction of oxophilic metal Bi can enhance adsorption of OHads,thereby significantly facilitating removal of poisoned intermediates.Density functional theory(DFT)simulations further indicate that formation of the PtBi intermetallic phase with the downshift of the Pt d-band center endows 3D Pt49.4Bi50.6 HASL intermetallics with significantly attenuated COads and enhanced OHads adsorption,bringing about the boosting electrocatalytic property.The mass activity of the 3D Pt49.4Bi50.6 HASL intermetallics for ethylene glycol oxidation reaction is as high as 24.67 A·mgPt^(−1),which is 12.98 times higher than that of commercial Pt/C(1.90 A·mgPt^(−1)).This work may inspire the design of Pt-based intermetallics as high-efficiency anode electrocatalysts for fuel cell applications.

关键词： surfactant-free strategy PtBi intermetallic three-dimensional hollow structure electrocatalyst ethylene glycol oxidation reaction

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