Ding Yubin, Li Xin, Hill Jonathan P, Ariga Katsuhiko, Agren Hans, Andréasson Joakim, Zhu Weihong, Tian He, Xie Yongshu
Key Laboratory for Advanced Materials and Institute of Fine Chemicals, Shanghai Key Laboratory of Functional Materials Chemistry, East China University of Science and Technology, Shanghai 200237 (P.R. China), Fax: (+86) 21-6425-2758.
Chemistry. 2014 Sep 26;20(40):12910-6. doi: 10.1002/chem.201403830. Epub 2014 Aug 14.
Compared with most of the reported logic devices based on the supramolecular approach, systems based on individual molecules can avoid challenging construction requirements. Herein, a novel dioxoporphyrin DPH22 was synthesized and two of its tautomers were characterized by single-crystal X-ray diffraction studies. Compound DPH22 exhibits multichannel controllable stepwise tautomerization, protonation, and deprotonation processes through interactions with H(+) and F(-) ions. By using the addition of H(+) and F(-) ions as inputs and UV/Vis absorption values at λ=412, 510, 562, and 603 nm as outputs, the controlled tautomerism of DPH22 has been successfully used for the construction of an integrated molecular level half-subtractor and comparator. In addition, this acid/base-switched tautomerism is reversible, thus endowing the system with ease of reset and recycling; consequently, there is no need to modulate complicated intermolecular interactions and electron-/charge-transfer processes.
与大多数已报道的基于超分子方法的逻辑器件相比，基于单个分子的系统可以避免具有挑战性的构建要求。在此，合成了一种新型二氧代卟啉DPH22，并通过单晶X射线衍射研究对其两种互变异构体进行了表征。化合物DPH22通过与H(+)和F(-)离子的相互作用，表现出多通道可控的逐步互变异构、质子化和去质子化过程。通过将H(+)和F(-)离子的添加作为输入，将λ=412、510、562和603 nm处的紫外/可见吸收值作为输出，DPH22的可控互变异构已成功用于构建集成分子水平半减法器和比较器。此外，这种酸/碱切换的互变异构是可逆的，从而使系统易于重置和循环利用；因此，无需调节复杂的分子间相互作用以及电子/电荷转移过程。
