Single-atom photocatalysts exhibit great potential for converting solar energy into value-added chemicals or fuels, but the insufficient efficiency of charge transfer from light-absorbed units to single-atom catalytic sites limits the overall photocatalytic performance. Herein, we developed an amorphization strategy of ferric oxide support to accelerate the enrichment of photogenerated electrons to single-atom Ru for enhanced nitrogen photofixation. The ammonia yield rate of Ru single atoms distributed on amorphous ferric oxide nanosheets (Ru₁/2DAF) in pure water reached 213 μmol·g_cat.^–1·h^–1, even four times higher than that of the crystalline counterpart. Mechanistic studies indicated that the amorphous structure could efficiently modulate the electronic density of states to reduce the electron-transfer energy barrier and guide electrons from amorphous support to Ru 4d orbitals via d(Ru)–d(Fe) coupling. This work provides fresh insights on the design of single-atom photocatalysts and emphasizes the importance of the charge transfer behavior in tuning the catalytic activity.

中文翻译：

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支持非晶化工程调节单原子钌作为氮光固定的电子泵

单原子光催化剂在将太阳能转化为增值化学品或燃料方面表现出巨大的潜力，但是从光吸收单元到单原子催化位点的电荷转移效率不足限制了整体光催化性能。在此，我们开发了一种氧化铁载体的非晶化策略，以加速光生电子向单原子 Ru 的富集，从而增强氮的光固定作用。纯水中分布在无定形氧化铁纳米片(Ru _{1 /2DAF)上的Ru单原子氨产率达到213 μmol·g cat。}^–1 ·h ^–1，甚至比结晶对应物高四倍。机理研究表明，无定形结构可以有效地调节电子态密度，从而降低电子转移能垒，并通过 d(Ru)-d(Fe) 耦合将电子从无定形载体引导到 Ru 4d 轨道。这项工作为单原子光催化剂的设计提供了新的见解，并强调了电荷转移行为在调节催化活性中的重要性。