The utilization of photocatalytic oxidation technology for sustainable production of value-added chemicals has garnered significant attention. In the photocatalytic process, the transfer rate of photogenerated holes is considerably slower (2–3 orders of magnitude) than that of electrons. Consequently, the migration of photogenerated holes emerges as a critical bottleneck in achieving the efficient conversion of solar energy into value-added chemicals. To address these challenges, we synthesized a perylene diimides supramolecule with abundant oxygen vacancies (R-Ov-PDI) to enhance holes transfer processes. Photogenerated holes were selectively captured by negatively charged defect sites, triggering an attack on the C–N bond. Noticeably, the catalyst exhibited a remarkable benzylamine oxidation efficiency (31.3 mmol·g·h) under visible light, with a selectivity for imine surpassing 99%. Furthermore, it demonstrated excellent substrate generality, outperforming most reported all-organic photocatalysts by 1–2 orders of magnitude. This study prove a novel perspective for the systematic design of efficient organic photocatalysts.

中文翻译：

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氧空位苝二酰亚胺超分子高效光催化将胺转化为亚胺

利用光催化氧化技术可持续生产高附加值化学品已引起人们的广泛关注。在光催化过程中，光生空穴的传输速率比电子的传输速率慢得多（2-3个数量级）。因此，光生空穴的迁移成为实现太阳能有效转化为增值化学品的关键瓶颈。为了应对这些挑战，我们合成了一种具有丰富氧空位的苝二酰亚胺超分子（R-Ov-PDI）来增强空穴传输过程。光生空穴被带负电的缺陷位点选择性捕获，引发对 C-N 键的攻击。值得注意的是，该催化剂在可见光下表现出显着的苄胺氧化效率（31.3 mmol·g·h），亚胺选择性超过99%。此外，它表现出出色的底物通用性，比大多数报道的全有机光催化剂高出 1-2 个数量级。这项研究为高效有机光催化剂的系统设计提供了新的视角。