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Reconstructed Vanadium Carbide MXene-Supported Cerium-Based Trimetallic Phosphide as an Efficient Electrocatalyst for Alkaline Water Splitting
重構型釩碳化物MXene支撐鈰基三金屬磷化物於鹼性水分解之高效電催化劑


Yu-Han Pan, Sakthivel Perumal, Mani Sakthivel, Shan-Ni Lin, Min-Hsin Yeh*, Wen-Yueh Yu b, Kuo-Chuan Ho
https://doi.org/10.1016/j.cej.2025.163888
SEED Member: Min-Hsin Yeh

 

Schematic illustration.

 

Major Contributions

1. Development of a Novel Trimetallic Phosphide/MXene Heterostructure Electrocatalyst
A simple and effective synthesis strategy was established to create a cerium-based trimetallic phosphide (CeCoFeP) integrated with V₂C MXene, resulting in a unique heterostructure. This design leverages the high conductivity and tunable surface chemistry of MXene, combined with the redox flexibility of cerium and the catalytic synergy of cobalt and iron phosphides, to form a robust electrocatalyst for alkaline water splitting.

2. Outstanding Electrocatalytic Performance and Durability
The optimized CeCoFeP@MXene catalyst demonstrated remarkable bifunctional activity, requiring only 91 mV and 266 mV overpotential to achieve 10 mA cm⁻² for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. The assembled electrolyzer operated at a low cell voltage of 1.63 V for 10 mA cm⁻² and maintained excellent stability over 120 hours, outperforming many conventional and previously reported catalysts in both efficiency and operational lifespan.

3. Mechanistic Insights into Active Site Reconstruction and Synergistic Effects
Comprehensive post-catalysis characterization revealed that the true active sites for HER and OER are dynamically reconstructed phosphate-containing metal hydroxides and oxyhydroxides formed in situ during operation. The study elucidated how the interplay among Ce, Co, and Fe elements, phosphate stabilization, and the conductive MXene scaffold collectively enhance charge transfer, optimize intermediate adsorption, and sustain high catalytic activity under alkaline conditions.




主要貢獻

1. 創新三金屬磷化物/MXene異質結構電催化劑的開發
本研究建立了一套簡單有效的合成策略,製備出以釩碳化物MXene為載體的鈰基三金屬磷化物(CeCoFeP)異質結構。此設計結合了MXene的高導電性與可調表面化學、鈰的氧化還原靈活性,以及鈷、鐵磷化物的催化協同效應,形成適用於鹼性水分解的高效電催化劑。

2. 優異的雙功能電催化性能與耐久性
經優化的CeCoFeP@MXene催化劑展現出卓越的雙功能活性,在氫析出反應(HER)與氧析出反應(OER)中,分別僅需91 mV與266 mV的過電位即可達到10 mA cm⁻²的電流密度。組裝的電解槽於10 mA cm⁻²時只需1.63 V的低電壓,並能在120小時內維持極佳穩定性,無論效率或長期操作壽命均超越多數傳統與文獻報導的催化劑。

3. 活性位點重構與協同效應的機理洞察
透過全面的催化後表徵,證實HER與OER的真實活性位點為反應過程中原位生成的含磷金屬氫氧化物及氧氫化物。研究深入解析了鈰、鈷、鐵三元素間的協同作用、磷酸鹽穩定化與MXene高導電骨架如何共同提升電荷轉移、優化中間體吸附,並在鹼性條件下維持高催化活性。