Mechanistic Probes of Zeolitic Imidazolate Framework for Photocatalytic Application

Pattengale, Brian; Yang, Sizhuo; Lee, Sungsik; Huang, Jier

doi:10.1021/acscatal.7b02467

Title: Mechanistic Probes of Zeolitic Imidazolate Framework for Photocatalytic Application

Journal Article · Thu Nov 02 00:00:00 EDT 2017 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b02467· OSTI ID:1416007

^[1]; Yang, Sizhuo ^[1]; Lee, Sungsik ^[2];

^[1]

Marquette Univ., Milwaukee, WI (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division

In this work, we report a zeolitic imidazolate framework (ZIF-67) with remarkable activity for hydrogen evolution reaction (HER) of 40,500 μmol H²/g MOF, which is, to the best of our knowledge, the highest activity achieved by any MOF system. This result necessitated assessment of its atomic-scale mechanistic function for HER using advanced spectroscopy techniques including time-resolved optical (OTA) and in situ X-ray absorption (XAS) spectroscopy. Through the correlation of OTA results with catalytic performance, we demonstrated that the electron transfer (ET) rather than energy transfer (ENT) pathway between photosensitizer and ZIF-67 is the key factor that controls the efficiency of HER activity, as HER activity that undergoes ET pathway is 3 orders of magnitude higher than that of ENT process. Here, using in situ XAS, we unraveled the spectral features for key intermediate species which are likely responsible for the rate determining process under turn over conditions. Finally, this work represents an original approach to study porous ZIF materials at the molecular level using advanced spectroscopic techniques, providing unprecedented insights into the photoactive nature of ZIF frameworks.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1416007

Journal Information:: ACS Catalysis, Vol. 7, Issue 12; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 40 works

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Title: Mechanistic Probes of Zeolitic Imidazolate Framework for Photocatalytic Application

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