Multi-factor interfacial microenvironment regulation by 3DOM architecture

Major Contributions
 

1. Constructed a 3D ordered macroporous (3DOM) architecture from layered perovskite La₂CuO₄ that strengthens the surface electric field, elevates local pH and accelerates mass transport, driving complete reconstruction into dendritic grain-boundary-rich nano-copper.

2. Achieved a C₂₊ partial current density of 585 mA cm⁻² in a flow cell, outperforming the bulk counterpart and most reported Cu-oxide-based catalysts, and stable operation for ~200 h at 600 mA cm⁻² in a membrane-electrode assembly.

3. Identified undercoordinated, compressively strained Cu atoms at grain boundaries as active sites that facilitate *COH formation, stabilize *OCCOH and suppress H₂ evolution, establishing architecture-driven microenvironment engineering for CO₂RR catalyst design.

主要貢獻
 

1. 以層狀鈣鈦礦 La₂CuO₄ 建構三維有序大孔（3DOM）結構，同時增強表面電場、提高局部 pH 並加速質傳，驅動材料快速且完全重構為樹枝狀、富含晶界的奈米銅。

2. 於流動電解槽中達到 585 mA cm⁻² 的 C₂₊ 分電流密度，優於塊材對照組及多數已報導的氧化銅基觸媒；在膜電極組（MEA）中於 600 mA cm⁻² 穩定運轉約 200 小時，並維持高 C₂₊ 選擇性。

3. 結合實驗與理論計算，確認晶界上低配位且受壓縮應變的銅原子為 C₂₊ 生成的活性位點，可促進 *COH 生成、穩定 *OCCOH 中間體並抑制產氫副反應，建立以電極架構調控微環境的 CO₂RR 觸媒設計策略。