Polymeric carbon nitride (CN) is one of the most promising metal-free photocatalysts to alleviate the energy crisis and environmental pollution. Loading cocatalysts is regarded as an effective way to improve the photocatalytic efficiency of CNs. However, commonly used noble metal cocatalysts limit their applications due to their rarity and high cost. Herein, we present the effective synthesis of single-atom copper-modified CN via supramolecular preorganization with subsequent condensation, which provides effective charge transfer pathways by an “infused” delocalized state with variable-valence catalysis at the same time. The C–Cu–N₂ single-atom catalytic site can activate CO₂ molecules and reduces the energy barrier toward photocatalytic CO₂ reduction. Excellent performance for photocatalytic CO₂ reduction was found. This work thereby provides a general protocol of designing a noble-metal-free photocatalyst with infused metal centers toward a wide range of applications.

中文翻译：

---

单一的含酶模拟铜中心，能够在CO2还原下实现完全的光合作用。

聚合氮化碳（CN）是缓解能源危机和环境污染的最有前途的无金属光催化剂之一。负载助催化剂被认为是提高CNs光催化效率的有效方法。然而，由于稀有性和高成本，常用的贵金属助催化剂限制了它们的应用。在本文中，我们介绍了通过超分子预组织和随后的缩合反应有效合成单原子铜修饰的CN的方法，该方法通过“注入”离域状态同时具有可变价催化作用提供了有效的电荷转移途径。C–Cu–N ₂单原子催化位点可以激活CO ₂分子并减少对光催化CO ₂的能垒减少。发现了光催化还原CO _2的优异性能。因此，这项工作为设计具有广泛应用范围的设计了通用的方案，该方案设计了具有注入的金属中心的无贵金属光催化剂。