Engineering Structurally Ordered High-Entropy Intermetallic Nanoparticles with High-Activity Facets for Oxygen Reduction in Practical Fuel Cells,Journal of the American Chemical Society

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Engineering Structurally Ordered High-Entropy Intermetallic Nanoparticles with High-Activity Facets for Oxygen Reduction in Practical Fuel Cells
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-09 , DOI: 10.1021/jacs.3c00868
Guang Feng ₁ , Fanghua Ning ₁ , Yue Pan ₂ , Tao Chen ₁ , Jin Song ₁ , Yucheng Wang ₃ , Ruqiang Zou ₁ , Dong Su ₂ , Dingguo Xia _{1,

4}

Affiliation

High-entropy solid-solution alloys have generated significant interest in energy conversion technologies. However, structurally ordered high-entropy intermetallic (HEI) nanoparticles (NPs) have been rarely reported in electrocatalysis applications. Here, we demonstrate structurally ordered PtIrFeCoCu HEI (PIFCC-HEI) NPs with extremely superior performance for both oxygen reduction reaction (ORR) and H₂/O₂ fuel cells. The PIFCC-HEI NPs show an average diameter of 6 nm. Atomic structural characterizations including atomic-resolution energy-dispersive spectroscopy (EDS) mapping technology confirm the ordered intermetallic structure of PIFCC-HEI NPs. As an electrocatalyst for ORR, the PIFCC-HEI/C achieves an ultrahigh mass activity of 7.14 A mg_{noble metals}^–1 at 0.85 V and extraordinary durability over 60 000 potential cycles. Moreover, the fuel cell assembled with PIFCC-HEI/C as the cathode delivers an ultrahigh peak power density of 1.73 W cm^–2 at a back pressure of 1.0 bar and almost no working voltage decay after 80 h operation, certifying the top-level performance among reported fuel cells. Theoretical calculations combined with experimental results reveal that the superior performance of PIFCC-HEI/C for ORR and fuel cells is attributed to its ultrahigh-activity facets. Especially, the (001) facet affords the lowest activation barriers for the rate-limiting step, the optimal downshift of the d-band center, and more efficient regulation of electron structures for ORR. This work not only opens up a new avenue for the fabrication of high-activity facets in the catalysts but also highlights structurally ordered HEI NPs as sufficiently effective catalysts in practical fuel cells and other potential energy-related applications.

中文翻译：

工程结构有序的高熵金属间化合物纳米粒子，具有高活性小平面，用于实际燃料电池中的氧还原

高熵固溶体合金引起了人们对能量转换技术的极大兴趣。然而，在电催化应用中很少报道结构有序的高熵金属间化合物 (HEI) 纳米粒子 (NP)。在这里，我们展示了结构有序的 PtIrFeCoCu HEI (PIFCC-HEI) NPs，其在氧还原反应 (ORR) 和 H ₂ /O ₂燃料电池中均具有极其优异的性能。PIFCC-HEI NP 的平均直径为 6 nm。包括原子分辨率能量色散光谱 (EDS) 映射技术在内的原子结构表征证实了 PIFCC-HEI NP 的有序金属间结构。作为 ORR 的电催化剂，PIFCC-HEI/C 实现了 7.14 A mg_{贵金属的超高质量活性}^–1在 0.85 V 和超过 60 000 个潜在循环的非凡耐久性。此外，以 PIFCC-HEI/C 为阴极组装的燃料电池可提供 1.73 W cm ^{–2的超高峰值功率密度}在 1.0 bar 的背压下，运行 80 小时后几乎没有工作电压衰减，证明了已报道燃料电池中的顶级性能。理论计算与实验结果相结合表明，PIFCC-HEI/C 在 ORR 和燃料电池中的优异性能归因于其超高活性方面。特别是，(001) 面为限速步骤提供了最低的激活势垒、d 带中心的最佳下移以及对 ORR 电子结构的更有效调节。这项工作不仅为在催化剂中制造高活性面开辟了一条新途径，而且还强调了结构有序的 HEI NPs 在实际燃料电池和其他潜在能源相关应用中作为足够有效的催化剂。

更新日期：2023-05-09

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