Guest modulating the photoactivity of a titanium-oxide cage

IF 7.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Chemical Science Pub Date : 2024-11-13 DOI:10.1039/d4sc04983g

Dexin Wang, Yanshu Liu, Guanyun Zhang, Menghui Chu, Fangfang Gao, Guanjie Chen, Guo Wang, Chen-Ho Tung, Yifeng Wang

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Abstract

Two host–guest Ti-oxide clusters, Ti₁₄(NH₄)₂ and Ti₁₄Cs₂, were synthesized and thoroughly characterized. They possess a rarely seen biloculate structure that encapsulates two NH₄⁺ and Cs⁺ guests, respectively. Interestingly, alkali metal cations can exchange places with NH₄⁺. The ability of the host to capture the guest cations follows the order Cs⁺ > NH₄⁺ > Rb⁺ > K⁺. The guests heavily influence the physiochemical properties and photocatalytic activities of the complexes. Ti₁₄Cs₂ exhibits a redshifted visible-light absorption edge, increased charge-separation properties, and enhanced interfacial charge-transfer ability compared to Ti₁₄(NH₄)₂. It also demonstrates excellent performance in photocatalytic CO₂/epoxide cycloaddition reactions regarding the reaction rate, scalability, sunlight usage, catalyst recyclability, and stability. This study presents a novel Ti-oxide-based cage cluster with exchangeable guests and provides insights for enhancing the solar harvesting applications of Ti-oxide cages.

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调节氧化钛笼光活性的客人

我们合成了两种主-客氧化钛团簇 Ti14(NH4)2 和 Ti14Cs2，并对它们进行了全面的表征。它们具有罕见的双胞结构，分别包裹着两个 NH4+ 和 Cs+ 客体。有趣的是，碱金属阳离子可以与 NH4+ 交换位置。宿主捕获客体阳离子的能力按照 Cs+ > NH4+ > Rb+ > K+ 的顺序排列。客体对配合物的理化性质和光催化活性有很大影响。与 Ti14(NH4)2 相比，Ti14Cs2 的可见光吸收边红移、电荷分离性能提高、界面电荷转移能力增强，在光催化 CO2/环氧化物环加成反应中的反应速率、可扩展性、日光利用率、催化剂可回收性和稳定性等方面也表现出优异的性能。本研究提出了一种具有可交换客体的新型氧化钛笼簇，并为提高氧化钛笼簇的太阳能收集应用提供了启示。

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来源期刊

Chemical Science CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

4.80%

发文量

1352

审稿时长

2.1 months

期刊介绍： Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.