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Title: Fe‐Triazolate Metal–Organic Frameworks as Water Oxidation Catalysts with Dual Photoanode Functionality
Abstract Artificial photosynthesis is an emerging technology that achieves renewable fuels, such as hydrogen, from sunlight. Its realization depends on finding highly active and stable catalysts of water splitting and photoactive materials for light absorption. To be scalable, these should contain only abundant elements. Here, for the first time, Fe‐triazolate (Fe(ta)2) and its metal substituted derivatives (Fe‐Metal(ta)2) Metal‐organic frameworks (MOFs) are characterized as new dual‐function materials for photo‐absorption and water oxidation catalysis in acidic media. The materials were studied by a range of structural, spectroscopic, and computational density functional theory (DFT) techniques. Fe(ta)2and Fe‐Mn(ta)2were found to be highly active and stable in chemical and photochemical water oxidation, and in addition function as photoanodes, with photo‐electrocatalytic currents (∼2.00 x 10−3Acm−2at + 1.4 V vs. Ag/AgCl) atpH = 1. The possibility of a unique catalytic mechanism where O─O bond formation is possible from the coupling of two adjacent FeIV = O fragments was demonstrated by DFT analysis. Thus, Fe‐triazolate MOF has been established as a new, stable, scalable, versatile, and efficient platform for sustainable energy conversion in the realm of artificial photosynthesis.  more » « less
Award ID(s):
2155060
PAR ID:
10648760
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
German Chemical Society
Date Published:
Journal Name:
Angewandte Chemie
Volume:
137
Issue:
40
ISSN:
0044-8249
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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