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

Journal Article · Wed Jun 22 00:00:00 EDT 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b04615· OSTI ID:1390793

Pattengale, Brian ^[1]; Yang, Sizhuo ^[1]; Ludwig, John ^[1]; Huang, Zhuangqun ^[1]; Zhang, Xiaoyi ^[2]; Huang, Jier ^[1]

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1. Department of Chemistry, Marquette University, Milwaukee, Wisconsin 53201, United States
2. X-ray Science Division, Argonne National Laboratory, Argonne, Illinois 60349, United States

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-visible-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 state with ligandto-metal charge transfer character using XTA. The surprisingly long-lived charge separated state, together with its intrinsic hybrid nature, all point to its potential application in heterogeneous photocatalysis and energy conversion.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES); Marquette University
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1390793
• Journal Information: Journal of the American Chemical Society, Vol. 138, Issue 26; ISSN 0002-7863
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English