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通过共价锚定在还原氧化石墨烯上增强基于钌多吡啶的光催化剂的光稳定性和光活性。

Enhanced Photostability and Photoactivity of Ruthenium Polypyridyl-Based Photocatalysts by Covalently Anchoring Onto Reduced Graphene Oxide.

作者信息

Hennessey Seán, González-Gómez Roberto, McCarthy Kathryn, Burke Christopher S, Le Houérou Camille, Sarangi Nirod Kumar, McArdle Patrick, Keyes Tia E, Cucinotta Fabio, Farràs Pau

机构信息

School of Biological and Chemical Sciences, Energy Research Centre, Ryan Institute, University of Galway, H91 CF50 Galway, Ireland.

School of Chemical Sciences, National Centre for Sensor Research, Dublin City University, Dublin 9, Ireland.

出版信息

ACS Omega. 2024 Mar 14;9(12):13872-13882. doi: 10.1021/acsomega.3c08800. eCollection 2024 Mar 26.

Abstract

Recentstudies toward finding more efficient ruthenium metalloligands for photocatalysis applications have shown that the derivatives of the linear [Ru(dqp)] (dqp: 2,6-di(quinolin-8-yl)-pyridine) complexes hold significant promise due to their extended emission lifetime in the μs time scale while retaining comparable redox potential, extinction coefficients, and absorption profile in the visible region to [Ru(bpy)] (bpy: 2,2'-bipyridine) and [Ru(tpy)] (tpy: 2,2':6',2″-terpyridine) complexes. Nevertheless, its photostability in aqueous solution needs to be improved for its widespread use in photocatalysis. Carbon-based supports have arisen as potential solutions for improving photostability and photocatalytic activity, yet their effect greatly depends on the interaction of the metal complex with the support. Herein, we present a strategy for obtaining Ru-polypyridyl complexes covalently linked to aminated reduced graphene oxide (rGO) to generate novel materials with long-term photostability and increased photoactivity. Specifically, the hybrid Ru(dqp)@rGO system has shown excellent photostable behavior during 24 h of continual irradiation, with an enhancement of 10 and 15% of photocatalytic dye degradation in comparison with [Ru(dqp)] and Ru(tpy)@rGO, respectively, as well as remarkable recyclability. The presented strategy corroborates the potential of [Ru(dqp)] as an interesting photoactive molecule to produce more advantageous light-active materials by covalent attachment onto carbon-based supports.

摘要

近期,为寻找更高效的用于光催化应用的钌金属配体所开展的研究表明,线性[Ru(dqp)](dqp:2,6 - 二(喹啉 - 8 - 基)吡啶)配合物的衍生物具有显著前景,因为它们在微秒时间尺度上具有延长的发射寿命,同时在氧化还原电位、消光系数以及可见光区域的吸收光谱方面与[Ru(bpy)](bpy:2,2'-联吡啶)和[Ru(tpy)](tpy:2,2':6',2″-三联吡啶)配合物相当。然而,其在水溶液中的光稳定性需要提高,以便在光催化中广泛应用。碳基载体已成为提高光稳定性和光催化活性的潜在解决方案,但其效果很大程度上取决于金属配合物与载体之间的相互作用。在此,我们提出一种策略,用于获得与胺化还原氧化石墨烯(rGO)共价连接的钌 - 多吡啶配合物,以生成具有长期光稳定性和增强光活性的新型材料。具体而言,混合的Ru(dqp)@rGO体系在连续照射24小时期间表现出优异的光稳定行为,与[Ru(dqp)]和Ru(tpy)@rGO相比,光催化染料降解分别增强了10%和15%,并且具有显著的可回收性。所提出的策略证实了[Ru(dqp)]作为一种有趣的光活性分子,通过共价连接到碳基载体上以生产更具优势的光活性材料的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a587/10976380/1cc9ad602a44/ao3c08800_0001.jpg

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