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

Journal Article · · ACS Energy Letters
 [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

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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1425274
Journal Information:
ACS Energy Letters, Vol. 3, Issue 3; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 46 works
Citation information provided by
Web of Science

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Cited By (9)

A Reusable MOF-Supported Single-Site Zinc(II) Catalyst for Efficient Intramolecular Hydroamination of o -Alkynylanilines journal May 2019
1,10‐Phenanthroline Carboxylic Acids for Preparation of Functionalized Metal‐Organic Frameworks journal September 2019
A novel Zr-MOF-based and polyaniline-coated UIO-67@Se@PANI composite cathode for lithium–selenium batteries journal January 2019
A Reusable MOF‐Supported Single‐Site Zinc(II) Catalyst for Efficient Intramolecular Hydroamination of o ‐Alkynylanilines journal May 2019
Characterization of Photo-catalysts: From Traditional to Advanced Approaches journal August 2019
Strongly visible light-absorbing metal–organic frameworks functionalized by cyclometalated ruthenium( ii ) complexes journal January 2020
Heterometallic multinuclear nodes directing MOF electronic behavior journal January 2020
From IR to x-rays: gaining molecular level insights on metal-organic frameworks through spectroscopy journal August 2019
Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework journal August 2018

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