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▌Entropy-Stabilized Cation–Anion Vacancies Coupling in High-Entropy Two-Dimensional Crystals for Efficient Oxygen Evolution
熵穩定的陽離子–陰離子空位耦合於高熵二維晶體中實現高效析氧反應


Ning Sun, Zhichuan Zheng, Lan Jiang, Guowei Liu, Yang Qin, Wei-Hsiang Huang, Chih-Wen Pao, Zhiwei Hu, Ming Lei, Tianping Ying, Runze Yu* and Kai Huang*
https://doi.org/10.1002/adfm.75186
SEED Member: Wei-Hsiang Huang

 
Cation–anion vacancy coupling in high-entropy HE₀.₇PS₃₋δ
 

Major Contributions
 

1. Reported an entropy-stabilized cation–anion vacancy coupling strategy in high-entropy metal phosphorus trisulfides (MPS₃), enabling semi-quantitative control of coupled metal and sulfur vacancies within a single-phase lattice.

2. Operando Raman and DFT revealed that coupled vacancies promote earlier surface reconstruction with enhanced OH* adsorption while suppressing over-oxidation and metal dissolution, with vacancy-activated Co-centered edge motifs dominating OER kinetics.

3. HE₀.₇PS₃₋δ delivers 212 mV at 10 mA cm⁻², a Tafel slope of 28.6 mV dec⁻¹ and 800 h stability at 200 mA cm⁻²; in an alkaline electrolyzer it operates at 1.8 V at 1 A cm⁻² and runs 300 h at 0.5 A cm⁻².




主要貢獻
 

1. 提出熵穩定的陽離子–陰離子空位耦合策略,於高熵金屬磷三硫化物(MPS₃)單相晶格中半定量調控金屬與硫空位。

2. 臨場拉曼光譜與 DFT 計算顯示,耦合空位促使表面提早重構並增強 OH* 吸附,同時抑制過度氧化與金屬溶出;由空位活化的鈷中心邊緣位點主導析氧反應動力學。

3. HE₀.₇PS₃₋δ 於 10 mA cm⁻² 的過電位為 212 mV、Tafel 斜率 28.6 mV dec⁻¹,並在 200 mA cm⁻² 穩定 800 小時;組成鹼性電解槽後於 1 A cm⁻² 僅需 1.8 V,並在 0.5 A cm⁻² 運轉 300 小時。