Exceptionally Long-Lived Charge Separated State in Zeolitic Imidazolate Framework: Implication for Photocatalytic Applications

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• 作者：Brian Pattengale ; Sizhuo Yang ; John Ludwig ; Zhuangqun Huang ; Xiaoyi Zhang ; Jier Huang
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：July 6, 2016
• 年：2016
• 卷：138
• 期：26
• 页码：8072-8075
• 全文大小：358K
• 年卷期：0
• ISSN：1520-5126

文摘

Zeolitic imidazolate frameworks (ZIFs) have emerged as a novel class of porous metal–organic frameworks (MOFs) for catalysis application because of their exceptional thermal and chemical stability. Inspired by the broad absorption of ZIF-67 in UV–vis-near IR region, we explored its excited state and charge separation dynamics, properties essential for photocatalytic applications, using optical (OTA) and X-ray transient absorption (XTA) spectroscopy. OTA results show that an exceptionally long-lived excited state is formed after photoexcitation. This long-lived excited state was confirmed to be the charge-separated (CS) state with ligand-to-metal charge-transfer character using XTA. The surprisingly long-lived CS state, together with its intrinsic hybrid nature, all point to its potential application in heterogeneous photocatalysis and energy conversion.