Abstract
Opportunity to harmonize aspects of oxygen reduction reaction (ORR) performance and structure, and morphology, as well as composition, is urgent for the commercialization of proton exchange membrane fuel cells. Herein, we demonstrate the design and synthesis of a functionalized-supported-Pt catalyst (Pt@HNC) featuring a hollow nitrogen-modified dodecahedral carbon substrate obtained by a stress-induced-shrink tailoring route. The as-obtained Pt@HNC catalyst possesses enhanced ORR performance, in particular with half-wave potential, mass activity (MA) and specific activity, which greatly exceed the commercial Pt/C. The density functional theory (DFT) calculations further confirmed that the charge redistribution induced by the electronegativity differences improved the electron interaction between Pt and HNC support. The optimized electronic structure of Pt weakens the reaction energy barrier on the Pt@HNC surface and adsorption of *OH species, thus cooperatively improving the intrinsic activity toward ORR. Additionally, our work indeed provides a guide for the future design of functional nanomaterials in the field of catalysts and clean energy.
Graphical abstract
摘要
质子交换膜燃料电池 (PEMFC)的商业化迫切需要协调氧还原反应(ORR)性能、结构、形貌和组成等方面。在此,我们展示了一种通过应力诱导收缩定制路线制备的以中空氮修饰的十二面体碳基底为特点负载功能化Pt催化剂 (Pt@HNC) 的设计与合成。所获得的Pt@HNC催化剂展示了增强的氧还原反应性能,特别是半波电位,质量活性和面积活性,都超过商业Pt/C。密度泛函理论 (DFT)计算进一步证明由电负性差异诱导的电荷再分布增强了Pt与HNC载体的之间的电子相互作用。Pt电子结构的优化削弱了Pt@HNC表面的反应能垒和*OH物种的吸附,从而增强Pt@HNC催化剂对氧还原反应的内在活性。此外,我们的工作确实为未来在催化剂和清洁能源领域设计功能性纳米材料提供了指导。
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Acknowledgements
This study was financially supported by the Natural Science Foundation of China (Nos. 22169005, 22068009 and 22262006), the Natural Science Special Foundation of Guizhou University (Nos. 202017 Special Post A and 702775203301), the Science and Technology Support Project of Guizhou Provincial Science and Technology Department (Nos. ZK[2023]050, ZK[2023]403) and The Open Project of Institute of Dual-carbon and New Energy Technology Innovation and Development of Guizhou Province (No. DCRE-2023-06).
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Long, J., Zhuang, KW., Liao, W. et al. Electronegativity-assisted optimized electronic structure of functionalized-Pt catalysts for boosting oxygen reduction kinetics. Rare Met. 43, 1965–1976 (2024). https://doi.org/10.1007/s12598-023-02580-x
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DOI: https://doi.org/10.1007/s12598-023-02580-x