Self-condensed organometallo Ir(III) ionosilica for sustainable visible-light promoted electron-transfer photocatalysis

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-03-01 Epub Date: 2025-01-08 DOI:10.1016/j.jcat.2025.115946
Mónica Martínez-Aguirre , Janira Herce , Elena Serrano , Javier García-Martínez , Miguel A. Rodríguez , Jesús R. Berenguer
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Abstract

Visible light photocatalysis represents a powerful approach to advancing the principles of green chemistry. Consequently, there is considerable research interest in the development of novel photocatalysts that are not only highly active but also readily reusable. To this end, we report here the synthesis of a novel luminescent organometallo-ionosilica obtained by sol–gel reactions. This material consists of discrete nanoparticles composed entirely of cationic cyclometallated iridium(III) fragments and their corresponding PF6- counterions. This organometallo-ionosilica has been extensively tested as a photocatalyst under heterogeneous conditions in both reductive and oxidative single electron transfer deactivation reactions, achieving reaction yields of around 90% and retaining up to 80% of its efficiency after seven consecutive reuse cycles. These results demonstrate the potential of our self-condensation strategy to heterogenize photoactive complexes, while retaining their catalytic activity and showing excellent reusability.

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自凝聚有机金属Ir(III)离子二氧化硅可持续可见光促进电子转移光催化
可见光光催化是推进绿色化学原理的有力途径。因此,开发既具有高活性又易于重复使用的新型光催化剂具有重要的研究意义。为此,我们在此报道了一种新型发光有机金属离子二氧化硅的合成,该有机金属离子二氧化硅是通过溶胶-凝胶反应获得的。该材料由完全由阳离子环金属化铱(III)碎片及其相应的PF6-反离子组成的离散纳米颗粒组成。这种有机金属离子二氧化硅作为光催化剂在非均相条件下进行了广泛的测试,用于还原性和氧化性单电子转移失活反应,在连续7次重复使用循环后,反应收率约为90%,效率保持在80%。这些结果表明,我们的自缩合策略在保持光活性配合物的催化活性和具有良好的可重复使用性的同时,具有多相化光活性配合物的潜力。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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