Orthogonal Supramolecular Assembly Triggered by Inclusion and Exclusion Interactions with Cucurbit[7]uril for Photocatalytic H2 Evolution.,ChemSusChem

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Orthogonal Supramolecular Assembly Triggered by Inclusion and Exclusion Interactions with Cucurbit[7]uril for Photocatalytic H2 Evolution.
ChemSusChem ( IF 7.5 ) Pub Date : 2019-11-04 , DOI: 10.1002/cssc.201902668
Dengmeng Song ₁ , Bo Li ₂ , Xin Li ₂ , Xuzhuo Sun ₂ , Jun Li ₁ , Chengbo Li ₁ , Tongyu Xu ₁ , Yong Zhu ₃ , Fei Li ₃ , Ning Wang _{1,

3}

Affiliation

The fabrication of efficient and convenient photocatalytic H2 evolution systems is a fascinating research topic in the field of solar energy conversion. A ternary self-assembled photocatalytic H2 evolution system was fabricated through supramolecular host-guest chemistry. The system consisted of the H2 evolution catalyst [Co(dmgH)2 (4-ppy)2 ]NO3 (1; dmgH2 =dimethylglyoxime, 4-ppy=4-phenylpyridine) and the photosensitizer Eosin Y (EY) assembled with the macrocyclic compound cucurbit[7]uril (CB[7]) to form the 1@CB[7]/EY complex through inclusion and exclusion interactions, respectively. The synchronous self-assembly drives an orthogonal arrangement of the 1@CB[7]/EY system. The inclusion complex 1@CB[7] was successfully characterized by 1 H NMR spectroscopy and single-crystal XRD. The exclusion process of CB[7] with EY was identified by NMR titration and the optimized geometry of the exclusion structure was determined by DFT calculations. The use of CB[7] resulted in a 6-fold increase in turnover number, a 3-fold increase in turnover frequency, and a 3-fold extension of lifetime for photocatalytic H2 evolution as compared with the system in the absence of CB[7]. The improvement of the light-driven H2 evolution activity was ascribed to the ability of CB[7] to link the photosensitizer and catalyst.

中文翻译：

正交超分子组装由与葫芦[7]尿素的包涵和互斥相互作用触发，用于光催化H2的演化。

高效，便捷的光催化氢气释放系统的制造是太阳能转化领域一个引人入胜的研究主题。通过超分子主客体化学方法制备了三元自组装的光催化氢气释放系统。该系统由H2析出催化剂[Co（dmgH）2（4-ppy）2] NO3（1; dmgH2 =二甲基乙二肟，4-ppy = 4-苯基吡啶）和光敏剂曙红Y（EY）与大环化合物组装而成葫芦[7] uril（CB [7]）通过包含和排除相互作用分别形成1 @ CB [7] / EY复合物。同步自组装驱动1 @ CB [7] / EY系统的正交排列。包合物1 @ CB [7]通过1 H NMR光谱和单晶XRD成功表征。通过NMR滴定法确定了CB [7]与EY的排斥过程，并通过DFT计算确定了排斥结构的最佳几何形状。与不使用CB的系统相比，使用CB [7]导致光催化H2释放的转换数增加了6倍，转换频率增加了3倍，寿命延长了3倍。 7]。光驱氢气释放活性的提高归因于CB [7]连接光敏剂和催化剂的能力。

更新日期：2019-11-04

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