Elucidating Charge Separation Dynamics in a Hybrid Metal–Organic Framework Photocatalyst for Light-Driven H2 Evolution

Yang, Sizhuo; Fan, Donghua; Hu, Wenhui; Pattengale, Brian; Liu, Cunming; Zhang, Xiaoyi; Huang, Jier

doi:10.1021/acs.jpcc.8b00471

Title: Elucidating Charge Separation Dynamics in a Hybrid Metal–Organic Framework Photocatalyst for Light-Driven H₂ Evolution

Journal Article · 30 January 2018 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.8b00471 · OSTI ID:1461304

Yang, Sizhuo ^[1]; Fan, Donghua ^[2]; Hu, Wenhui ^[1]; Pattengale, Brian ^[1]; Liu, Cunming ^[3];

^[3];

^[1]

Marquette Univ., Milwaukee, WI (United States). Dept. of Chemistry
Wuyi Univ., Jiangmen (China). School of Applied Physics and Materials
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division

Metal organic frameworks (MOFs) have emerged as novel scaffolds for artificial photosynthesis due to their unique capability in incorporating homogeneous photosensitizer and catalyst to their robust heterogeneous matrix. Here, we report the charge separation dynamics between molecular Ru-photosensitizer and Pt-catalyst, both of which were successfully incorporated into a Zr-MOF that demonstrates excellent activity and stability for light-driven H₂ generation from water. Using optical transient absorption (OTA) spectroscopy, we show that charge separation in this hybrid MOF occurs via electron transfer (ET) from Ru-photosensitizer to Pt-catalyst. Using Pt L₃-edge X-ray transient absorption (XTA) spectroscopy, we observed the intermediate reduced Pt site, directly confirming the formation of charge separated state due to ET from Ru-photosensitizer and unraveling their key roles in photocatalysis.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); American Chemical Society Petroleum Research Fund (ACS PRF)

Grant/Contract Number:: AC02-06CH11357; DMR-1654140; 57503-DNI6

OSTI ID:: 1461304

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 6; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Elucidating Charge Separation Dynamics in a Hybrid Metal–Organic Framework Photocatalyst for Light-Driven H2 Evolution

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