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Phase-Controlled Pd–S Nanosheet Aerogels for Electrocatalytic Upgrading of Waste Plastics
相位可控的Pd–S奈米片氣凝膠於廢塑膠電催化升級中的應用


Liheng Guan, Zhen Huang, Ting Zhu, Zhenyu Wang, Wei-Hsiang Huang*,Chun-Chi Chang, Min-Hsin Yeh*, Silvio Osella, Nan Zhang, and Tianxi Liu
https://doi.org/10.1002/adfm.202500254
SEED Member: Wei-Hsiang Huang, Min-Hsin Yeh

 

Schematic illustration of the syntheses and structural models of Pd─S NAs.

 

Major Contributions
 

1.Developed a seed-mediated synthesis strategy to achieve phase-controlled Pd–S nanosheet aerogels (NAs), enabling precise modulation from ordered Pd4S to amorphous Pd1S structures, and systematically elucidated the relationship between crystal phase and electrocatalytic performance for the ethylene glycol oxidation reaction (EGOR).

2.Demonstrated that the ordered Pd3S NAs with a Pd4S phase exhibit superior electrocatalytic activity, selectivity, and durability toward EGOR, significantly outperforming both S-doped Pd9S NAs and amorphous Pd1S NAs, as well as commercial Pd/C, due to optimized atomic arrangement and electronic structure.

3.Combined advanced characterization and density functional theory (DFT) calculations to reveal that the ordered phase structure of Pd3S NAs promotes *CO oxidation, optimizes adsorption of key intermediates, lowers the reaction barrier in the potential-determining step, and facilitates selective conversion of ethylene glycol to glycolic acid, thus providing a new paradigm for phase engineering in electrocatalyst design.




主要貢獻
 

1.建立種子誘導合成策略,成功實現相位可控的Pd–S奈米片氣凝膠,能夠從有序的Pd4S相調控至非晶態Pd1S結構,並系統性揭示晶體相與乙二醇氧化反應(EGOR)電催化性能之間的關聯。

2.證明有序Pd3S奈米片氣凝膠(Pd4S相)在EGOR中展現出卓越的電催化活性、選擇性與耐久性,明顯優於S摻雜的Pd9S奈米片與非晶態Pd1S奈米片,以及商用Pd/C,這歸因於其最佳化的原子排列與電子結構。

3.結合先進材料表徵與密度泛函理論(DFT)計算,揭示有序相結構能促進*CO氧化、優化關鍵中間體的吸附、降低反應決定步驟的能障,並促進乙二醇選擇性轉化為乙醇酸,為電催化劑相工程設計提供新典範。