Potential synergy between Pt₂Ni₄ Atomic-Clusters, oxygen vacancies and adjacent Pd nanoparticles outperforms commercial Pt nanocatalyst in alkaline fuel cells
三元 Pt₂Ni₄ 原子團簇與氧空位及相鄰鈀奈米粒子的潛在協同效應優於商用鉑奈米觸媒應用於鹼性燃料電池
📄 英文摘要
The oxygen reduction reaction (ORR) is a key "showstopper" for the commercial viability of alkaline fuel cells (AFCs). In this study, we developed a ternary nanocatalyst (NC) coloaded with Pt₂Ni₄ atomic clusters and palladium (Pd) nanoparticles (NPs) on oxygen vacancies (OVs) enriched nickel hydroxide-support (henceforth denoted as NiPP). This material outperforms the commercial J.M.-Pt/C (20 wt%) catalyst by ~75 and ~38 times with exceptionally high mass activities (MA)s of 5050.3 mAmg⁻¹Pt and 952.3 mAmg⁻¹Pt at 0.85 V and 0.90 V vs RHE, respectively, in alkaline ORR (0.1 M KOH). The high structural reliability of the Pt₂Ni₄ endows the NiPP NC with outstanding durability, where it achieves an optimum MA of 5755.9 mAmg⁻¹Pt after 10 K cycles in an accelerated durability test (ADT) and retains the original performance up to 15 K cycles. Moreover, NiPP delivers an outstanding power density (339.1 mW cm⁻²) and short circuit current density (910.8 mA cm⁻²), which exceeds the commercial J.M.-Pt/C (174.9 mW cm⁻² and 720.4 mA cm⁻²) when serving as the cathodic catalyst in an AFC. The results suggest that the exceptional performance originates from the potential synergism between the neighbouring reaction sites of Pt₂Ni₄ (OV in Ni(OH)x and Pd NPs). During ORR, the Pt₂Ni₄ atomic clusters and OVs boost the O₂ splitting, while the adjacent Pd NPs promote the subsequent relocation of OH⁻ ions.
📄 中文摘要
氧還原反應（ORR）是鹼性燃料電池（AFC）商業化發展的關鍵瓶頸。本研究開發了一種三元奈米觸媒（NC），將 Pt₂Ni₄ 原子團簇與鈀（Pd）奈米粒子（NP）共同負載於富含氧空位（OV）的氫氧化鎳載體上（以下簡稱 NiPP）。在鹼性 ORR（0.1 M KOH）中，該材料於 0.85 V vs RHE 達到 5050.3 mAmg⁻¹Pt 的質量活性，於 0.90 V vs RHE 達到 952.3 mAmg⁻¹Pt，較商用 J.M.-Pt/C（20 wt%）觸媒分別高出約 75 倍及 38 倍。Pt₂Ni₄ 的高結構可靠性賦予 NiPP 卓越的耐久性，在 10,000 次加速耐久性測試（ADT）後達到 5755.9 mAmg⁻¹Pt 的最佳質量活性，並在 15,000 次循環內完整維持原始性能。此外，NiPP 作為 AFC 陰極觸媒時展現 339.1 mW cm⁻² 的峰值功率密度及 910.8 mA cm⁻² 的短路電流密度，均超越商用 J.M.-Pt/C（174.9 mW cm⁻² 及 720.4 mA cm⁻²）。研究結果表明，卓越性能源自於 Pt₂Ni₄ 原子團簇（Ni(OH)x 中的 OV 與相鄰 Pd NP）的相鄰反應位點之間的潛在協同作用：在 ORR 期間，Pt₂Ni₄ 原子團簇和 OV 促進 O₂ 斷裂，而相鄰的 Pd NP 則促進後續 OH⁻ 離子的遷移。
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