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Dipole field in nitrogen-enriched carbon nitride with external forces to boost the artificial photosynthesis of hydrogen peroxide
Nature Communications ( IF 14.7 ) Pub Date : 2023-09-16 , DOI: 10.1038/s41467-023-41522-0
Zhi Li 1 , Yuanyi Zhou 1 , Yingtang Zhou 2 , Kai Wang 3 , Yang Yun 4 , Shanyong Chen 1 , Wentao Jiao 5 , Li Chen 6 , Bo Zou 3 , Mingshan Zhu 1
Affiliation  

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 (C3N5) to harness photogenerated charge kinetics for hydrogen peroxide production is constructed. Here, C3N5 achieves a hydrogen peroxide photosynthesis rate of 3809.5 µmol g−1 h−1 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 C3N5, 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.



中文翻译:

富氮氮化碳偶极场外力促进过氧化氢人工光合作用

人工光合作用是有效生产过氧化氢的一种有前景的策略,但从本体到活性位点的不良定向电荷转移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(C 3 N 5)中偶极场驱动自发极化的新工艺,以利用光生电荷动力学生产过氧化氢。在此,C 3 N 5在模拟阳光和超声波力下实现了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C 3 N 5中三唑环引入了丰富的氮活性位点,从而带来了偶极场。该偶极场诱发自发极化场,加速向氮活性位点的快速定向电子转移过程,从而通过间接 2e -转移途径诱发鲍林型氧吸附,形成过氧化氢。这一创新概念利用偶极场来利用光生载流子的迁移和传输,为通过结构工程提高光合作用效率提供了一条新途径。

更新日期:2023-09-16
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