Engineering palladium-nickel alloy sites on N-doped reduced graphene oxide for enhanced catalytic hydrogenation of vanadium electrolytes
在氮摻雜還原氧化石墨烯上設計鈀鎳合金活性位點，以強化釩電解質的催化氫化
📄 英文摘要
High-performance, low-cost electrolyte production remains a significant challenge for the commercialization of all-vanadium redox flow batteries (VRFBs). Herein, we demonstrate a robust strategy to engineer palladium-nickel (PdNi) alloy active sites on nitrogen-doped reduced graphene oxide (NrGO) for the efficient catalytic hydrogenation of VO₂⁺ (V⁴⁺) to the V³·⁵⁺. The resulting PdNi/NrGO catalyst outperforms commercial Pd/C, driven by synergistic Pd-Ni electronic interactions and the structural advantages of the N-doped support, which prevent particle agglomeration and enhance charge transfer. Kinetic analysis reveals a remarkable turnover frequency (TOF) of 0.765 s⁻¹, enabling rapid and impurity-free electrolyte generation. Crucially, the synthesized V³·⁵⁺ electrolyte delivers superior VRFB performance, achieving average efficiency gains of 16.6% (Coulombic efficiency), 11.0% (Energy efficiency), and 11.0% (Voltage efficiency) relative to the commercial baseline, while maintaining stable operation over 100 charge-discharge cycles. Furthermore, this bimetallic approach reduces catalyst costs by approximately 45% relative to commercial Pd/C and up to 71% compared to high-loading Pt-based systems.
📄 中文摘要
高效能且低成本的電解質製備，仍是全釩氧化還原液流電池（VRFBs）商業化的一道重大關卡。本研究提出一項強健的策略：在氮摻雜還原氧化石墨烯（NrGO）上構築鈀鎳（PdNi）合金活性位點，用於將 VO²⁺（V⁴⁺）高效催化氫化為 V³·⁵⁺。所製備的 PdNi/NrGO 催化劑之所以能超越商業 Pd/C，歸功於 Pd-Ni 之間的電子協同交互作用，以及氮摻雜載體在防止粒子團聚、促進電荷傳遞方面的結構優勢。動力學分析顯示，轉化頻率（TOF）高達 0.765 s⁻¹，能快速且無雜質地生成電解質。關鍵在於：以此 V³·⁵⁺ 電解質組裝的 VRFB 展現出優異性能——相較於商業基準，庫倫效率平均提升 16.6%、能量效率提升 11.0%、電壓效率提升 11.0%，並在 100 次充放電循環中維持穩定運作。此外，雙金屬策略使催化劑成本較商業 Pd/C 降低約 45%，較高載量鉑（Pt）系統更降低達 71%，為下一代電網儲能系統中的電解質不平衡問題，提供了一種可擴充且具經濟吸引力的解決方案。
🔬 五項核心重要發現
📊 關鍵圖表
