Sheng Yuqiang, Li Wenlu, Xu Liangliang, Zhu Yongfa
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
CTBT Beijing National Data Centre and Beijing Radionuclide Laboratory, Beijing, 100085, P. R. China.
Adv Mater. 2022 Mar;34(10):e2102354. doi: 10.1002/adma.202102354. Epub 2022 Jan 31.
A highly crystalline perylene imide supramolecular photocatalyst (PDI-NH) is synthesized via imidazole solvent method. The catalyst shows a breakthrough oxygen evolution rate (40.6 mmol g h ) with apparent quantum yield of 10.4% at 400 nm, which is 1353 times higher than the low crystalline PDI-NH. The highly crystalline structure comes from the ordered self-assembly process in molten imidazole solvent via π-π stacking and hydrogen bonding. Further, the excellent performance ascribes to the robust built-in electric field induced by its high crystallinity, which greatly accelerates the charge separation and transfer. What is more, the PDI-NH is quite stable and can be reused over 50 h without performance attenuation. Briefly, the crystalline PDI-NH with strong built-in electric field throws light on photocatalytic oxygen evolution, showing a new perspective for the design of organic photocatalysts.
通过咪唑溶剂法合成了一种高度结晶的苝酰亚胺超分子光催化剂(PDI-NH)。该催化剂表现出突破性的析氧速率(40.6 mmol g⁻¹ h⁻¹),在400 nm处的表观量子产率为10.4%,这比低结晶度的PDI-NH高1353倍。高度结晶的结构源于熔融咪唑溶剂中通过π-π堆积和氢键进行的有序自组装过程。此外,其优异的性能归因于由高结晶度诱导的强大内建电场,这极大地加速了电荷分离和转移。更重要的是,PDI-NH非常稳定,可以重复使用超过50小时而不衰减性能。简而言之,具有强内建电场的结晶PDI-NH为光催化析氧提供了启示,为有机光催化剂的设计展示了新的视角。