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Reactivity and Mechanisms of Photoactivated Heterometallic [Ru II Ni II ] and [Ru II Ni II Ru II ] Catalysts for Dihydrogen Generation from Water
Author(s) -
El Harakeh Nour,
Morais Ana C. P.,
Rani Neha,
Gomez Javier A. G.,
Cousino Abigail,
Lanznaster Mauricio,
Mazumder Shivnath,
Verani Cláudio N.
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202013678
Subject(s) - catalysis , bimetallic strip , chemistry , ruthenium , reactivity (psychology) , intramolecular force , photocatalysis , nickel , photochemistry , medicinal chemistry , crystallography , stereochemistry , medicine , biochemistry , alternative medicine , organic chemistry , pathology
Two heterometallic photocatalysts were designed and probed for water reduction. Both [(bpy) 2 Ru II Ni II (L 1 )](ClO 4 ) 2 ( 1 ) and [(bpy) 2 Ru II Ni II (L 2 ) 2 Ru II (bpy) 2 ](ClO 4 ) 2 ( 2 ) can generate the low‐valent precursor involved in hydride formation prior to dihydrogen generation. However, while the bimetallic [Ru II Ni II ] ( 1 ) requires the presence of an external photosensitizer to trigger catalytic activity, the trimetallic [Ru II Ni II Ru II ] ( 2 ) displays significant coupling between the catalytic and light‐harvesting units to promote intramolecular multielectron transfer and perform photocatalysis at the Ni center. A concerted experimental and theoretical effort proposes mechanisms to explain why 1 is unable to achieve self‐supported catalysis, while 2 is fully photocatalytic.
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