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Thermostable Tellurium Anchoring Enabling Robust Thermal and Electrochemical Stability for Pt3Co Intermetallic Fuel Cell Catalysts
Advanced Functional Materials ( IF 19 ) Pub Date : 2024-08-10 , DOI: 10.1002/adfm.202408383
Yuanxin Chen Zihan Meng Fei Liu Aojie Zhang Xiaocan Wang Yifei Xiong Haibo Tang Tian Tian Haolin Tang

Highly active Pt-based intermetallic nanoparticles (i-NPs) loaded on stable supports have garnered considerable interest as promising oxygen reduction reaction (ORR) catalysts for proton-exchange-membrane fuel cells (PEMFCs). Herein, thermostable tellurium (Te) is vapor-deposited onto commercial conductive carbon to anchor high-temperature-synthesized Pt3Co i-NPs. Advanced characterization and density functional theory (DFT) calculations demonstrate that the binding energy of Pt 4f and Co 2p shift positively by 0.12 and 0.95 eV after the introduction of Te in carbon support, promoting the formation of Pt─Te bonds, which enhances the metal–support interactions (MSIs) in Pt3Co/Te-C (with a more negative binding energy of −10.28 eV). The average size of well-dispersed Pt3Co i-NPs (≈3.9 nm) on Te─C is considerably smaller than that of Pt3Co i-NPs (≈9.1 nm) on commercial carbon. The specific activity of Pt3Co/Te-C decreases by only 1.5% after 100,000 ultra-long voltage-accelerated cycles, while the morphology remains almost unchanged. The membrane electrode assembly using Pt3Co/Te-C as a cathode demonstrates impressive activity (power density of 2.32 W cm−2@4 A cm−2 and mass activity of 0.50 A mgPt−1@0.9 V) and robust durability (mass activity@0.9 V loss of 26% after 30,000 cycles with intact L12 ordered structure) in H2–O2 operation, significantly exceeding the DOE 2025 requirements.

中文翻译:


热稳定碲锚定为 Pt3Co 金属间化合物燃料电池催化剂提供强大的热稳定性和电化学稳定性



负载在稳定载体上的高活性 Pt 基金属间化合物纳米颗粒 (i-NPs) 作为用于质子交换膜燃料电池 (PEMFC) 的有前途的氧还原反应 (ORR) 催化剂,引起了人们的极大兴趣。在此,热稳定碲 (Te) 被气相沉积到商业导电碳上,以锚定高温合成的 Pt3Co i-NPs。先进的表征和密度泛函理论 (DFT) 计算表明,在碳载体中引入 Te 后,Pt 4f 和 Co 2p 的结合能分别发生 0.12 和 0.95 eV 的正向移动,促进 Pt─Te 键的形成,从而增强 Pt3Co/Te-C 中的金属-载体相互作用 (MSI)(具有 -10.28 eV 的负结合能)。Te─C 上分散良好的 Pt3Co i-NPs (≈3.9 nm) 的平均尺寸比商业碳上的 Pt3Co i-NPs (≈9.1 nm) 小得多。Pt3Co/Te-C 的比活性在 100,000 次超长电压加速循环后仅下降了 1.5%,而形貌几乎保持不变。使用 Pt3Co/Te-C 作为阴极的膜电极组件在 H2–O2 操作中表现出令人印象深刻的活性(功率密度为 2.32 W cm-2@4 A cm-2,质量活性为 0.50 A mg Pt-1@0.9 V)和强大的耐用性(在完整的 L12 有序结构下,在 30,000 次循环后质量损失 activity@0.9 V 损失 26%), 大大超过了 DOE 2025 的要求。
更新日期:2024-08-10
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