Developing low-cost Cu-based photocatalysts is a promising strategy to boost catalytic activity for nitrogen (N₂) photofixation, but it remains a challenge. Herein, we successfully applied porous CuFe to construct plasmon-assisted Cu-based photocatalysts in N₂ photofixation via plasmonic catalysis. Surface Fe atoms were regarded as the active sites to efficiently adsorb and activate N₂, while Cu frameworks generated hot electrons by surface plasmon resonance (SPR). Impressively, porous Cu₉₆Fe₄ attained an NH₃ production rate of 342 μmol·g_cat.^–1·h^–1 in N₂ photofixation without any sacrificial agents. More importantly, porous Cu₉₆Fe₄ also displayed excellent stability by maintaining ∼100% initial activity after 10 cycles. Further mechanistic studies revealed that the valence state and coordination numbers of Fe atoms in porous Cu₉₆Fe₄ increased during catalytic process, indicating the formation of a surface nitrogen-containing complex. In addition, the reaction barrier significantly decreased because of the efficient polarization of N₂ over Fe atoms.

中文翻译：

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多孔CuFe用于等离子辅助N ₂光固定

开发低成本的基于铜的光催化剂是提高氮（N ₂）光固定催化活性的一种有前途的策略，但它仍然是一个挑战。在本文中，我们成功地将多孔CuFe应用于通过等离激元催化在N ₂光固定中构建等离激元辅助的Cu基光催化剂。表面的Fe原子被视为有效吸附和激活N ₂的活性位点，而Cu骨架则通过表面等离振子共振（SPR）产生热电子。令人印象深刻的是，多孔Cu ₉₆ Fe ₄的NH ₃产生率为342μmol·g _cat。^–1 ·h ^–1在N _2中没有任何牺牲剂的光固定。更重要的是，多孔Cu ₉₆ Fe ₄通过在10个循环后保持约100％的初始活性，也表现出出色的稳定性。进一步的机理研究表明，多孔Cu ₉₆ Fe _4中的Fe原子的价态和配位数在催化过程中增加，表明形成了表面含氮配合物。另外，由于N ₂在Fe原子上的有效极化，反应势垒显着降低。