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Title: Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst

Here in this work, we report a new single-site photocatalyst (Co-Ru-UIO- 67(bpy)) based on a metal-organic framework platform with incorporated molecular photosensitizer and catalyst. We show that this catalyst not only demonstrates exceptional activity for light-driven H 2 production but also can be recycled without loss of activity. Using the combination of optical transient absorption spectroscopy and in situ X-ray absorption spectroscopy, we not only captured the key Co I intermediate species formed after ultrafast charge transfer from the incorporated photosensitizer but also identified the rate-limiting step in the catalytic cycle, providing insight into the catalysis mechanism of these single-site metal-organic framework photocatalysts.
Authors:
 [1] ;  [1] ;  [2] ; ORCiD logo [1]
  1. Marquette Univ., Milwaukee, WI (United States). Dept. of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 3; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1425274

Yang, Sizhuo, Pattengale, Brian, Lee, Sungsik, and Huang, Jier. Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst. United States: N. p., Web. doi:10.1021/acsenergylett.8b00062.
Yang, Sizhuo, Pattengale, Brian, Lee, Sungsik, & Huang, Jier. Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst. United States. doi:10.1021/acsenergylett.8b00062.
Yang, Sizhuo, Pattengale, Brian, Lee, Sungsik, and Huang, Jier. 2018. "Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst". United States. doi:10.1021/acsenergylett.8b00062.
@article{osti_1425274,
title = {Real-Time Visualization of Active Species in a Single-Site Metal–Organic Framework Photocatalyst},
author = {Yang, Sizhuo and Pattengale, Brian and Lee, Sungsik and Huang, Jier},
abstractNote = {Here in this work, we report a new single-site photocatalyst (Co-Ru-UIO- 67(bpy)) based on a metal-organic framework platform with incorporated molecular photosensitizer and catalyst. We show that this catalyst not only demonstrates exceptional activity for light-driven H2 production but also can be recycled without loss of activity. Using the combination of optical transient absorption spectroscopy and in situ X-ray absorption spectroscopy, we not only captured the key CoI intermediate species formed after ultrafast charge transfer from the incorporated photosensitizer but also identified the rate-limiting step in the catalytic cycle, providing insight into the catalysis mechanism of these single-site metal-organic framework photocatalysts.},
doi = {10.1021/acsenergylett.8b00062},
journal = {ACS Energy Letters},
number = 3,
volume = 3,
place = {United States},
year = {2018},
month = {2}
}