Li Zhi, Zhou Yuanyi, Zhou Yingtang, Wang Kai, Yun Yang, Chen Shanyong, Jiao Wentao, Chen Li, Zou Bo, Zhu Mingshan
Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, 511443, Guangzhou, China.
Marine Science and Technology College, Zhejiang Ocean University, 316004, Zhoushan, China.
Nat Commun. 2023 Sep 16;14(1):5742. doi: 10.1038/s41467-023-41522-0.
Artificial photosynthesis is a promising strategy for efficient hydrogen peroxide production, but the poor directional charge transfer from bulk to active sites restricts the overall photocatalytic efficiency. To address this, a new process of dipole field-driven spontaneous polarization in nitrogen-rich triazole-based carbon nitride (CN) to harness photogenerated charge kinetics for hydrogen peroxide production is constructed. Here, CN achieves a hydrogen peroxide photosynthesis rate of 3809.5 µmol g h and a 2e transfer selectivity of 92% under simulated sunlight and ultrasonic forces. This high performance is attributed to the introduction of rich nitrogen active sites of the triazole ring in CN, which brings a dipole field. This dipole field induces a spontaneous polarization field to accelerate a rapid directional electron transfer process to nitrogen active sites and therefore induces Pauling-type adsorption of oxygen through an indirect 2e transfer pathway to form hydrogen peroxide. This innovative concept using a dipole field to harness the migration and transport of photogenerated carriers provides a new route to improve photosynthesis efficiency via structural engineering.
人工光合作用是一种很有前景的高效生产过氧化氢的策略，但从本体到活性位点的定向电荷转移较差，限制了整体光催化效率。为了解决这个问题，构建了一种在富氮三唑基氮化碳（CN）中由偶极场驱动的自发极化新过程，以利用光生电荷动力学来生产过氧化氢。在此，CN在模拟阳光和超声力作用下实现了3809.5 µmol g⁻¹ h⁻¹的过氧化氢光合作用速率和92%的2e转移选择性。这种高性能归因于CN中三唑环引入了丰富的氮活性位点，从而产生了偶极场。该偶极场诱导自发极化场，加速快速定向电子转移过程至氮活性位点，进而通过间接2e转移途径诱导氧的鲍林型吸附以形成过氧化氢。这种利用偶极场来控制光生载流子迁移和传输的创新概念，为通过结构工程提高光合作用效率提供了一条新途径。
