Wang Jiu, Heil Tobias, Zhu Bicheng, Tung Ching-Wei, Yu Jiaguo, Chen Hao Ming, Antonietti Markus, Cao Shaowen
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 Wuhan, People's Republic of China.
Department of Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, 14476 Potsdam, Germany.
ACS Nano. 2020 Jul 28;14(7):8584-8593. doi: 10.1021/acsnano.0c02940. Epub 2020 Jul 7.
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 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-N single-atom catalytic site can activate CO molecules and reduces the energy barrier toward photocatalytic CO reduction. Excellent performance for photocatalytic CO 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.
聚合氮化碳（CN）是最有前途的无金属光催化剂之一，可缓解能源危机和环境污染。负载助催化剂被认为是提高CN光催化效率的有效方法。然而，常用的贵金属助催化剂由于其稀有性和高成本限制了它们的应用。在此，我们展示了通过后续缩合有效合成单原子铜修饰的CN超分子预组装体，其通过“注入”离域态同时进行可变价催化提供了有效的电荷转移途径。C-Cu-N单原子催化位点可以激活CO分子并降低光催化CO还原的能量势垒。发现了光催化CO还原的优异性能。因此，这项工作提供了一种通用方案，用于设计具有注入金属中心的无贵金属光催化剂，以实现广泛的应用。
