Long-lived triplet excited states have been regarded as active species in the implementation of photochemical strategies owing to their associated high energy and electron transfer abilities, yet it was still challenging to fulfill this in polymeric photocatalysis. Herein, we formulated a built-in donor–acceptor interaction control strategy to prolong the excited-state lifetime in conjugated organic polymers (COPs) by minimizing the exciton binding energy in the first excited state. The resultant COPs decorated with tris([1,2,4]triazolo)[4,3-a:4′,3′-c:4′’,3′’-e][1,3,5]triazine exhibited excellent activities in photocatalytic amide formation (95 % yield), which was much higher than that of triazine rings as an analogous moiety(66 % yield) owing to its prolonged triplet-state lifetimes (τ = 30.5 µs) and the improved photo-induced charge separation efficiency. These results not only demonstrate the feasibility of realizing triplet excited states for heterogeneous photocatalysis through molecular engineering but also offers insights into energy and electron transfer at the molecular level.

中文翻译：

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延长三重态寿命，以促进共轭有机聚合物中的能量和电子转移，从而形成光催化酰胺


长寿命的三重态激发态因其相关的高能量和电子转移能力而被视为光化学策略实施中的活性物质，但在聚合物光催化中实现这一点仍然具有挑战性。在此，我们制定了一种内置的供体-受体相互作用控制策略，通过最小化第一激发态中的激子结合能来延长共轭有机聚合物 （COPs） 中的激发态寿命。用三嗪（[1,2,4]三唑并）[4,3-a：4′，3′-c：4′'，3′'-e][1,3,5]三嗪修饰的 COPs 在光催化酰胺形成中表现出优异的活性（95% 产率），远高于三嗪环作为类似部分的三嗪环（66% 产率），因为它延长了三重态寿命 （τ = 30.5 μs） 和提高了光诱导电荷分离效率。这些结果不仅证明了通过分子工程实现多相光催化的三重态激发态的可行性，而且为分子水平的能量和电子转移提供了见解。