Reactivity and Mechanisms of Photoactivated Heterometallic [RuIINiII] and [RuIINiIIRuII] Catalysts for Dihydrogen Generation from Water
Dr. Nour El Harakeh
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
These authors contributed equally to this work.
Search for more papers by this authorDr. Ana C. P. de Morais
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
These authors contributed equally to this work.
Search for more papers by this authorNeha Rani
Department of Chemistry, Indian Institute of Technology Jammu, Jammu, 181221 India
These authors contributed equally to this work.
Search for more papers by this authorDr. Javier A. G. Gomez
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
Search for more papers by this authorAbigail Cousino
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
Search for more papers by this authorCorresponding Author
Prof. Mauricio Lanznaster
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
Search for more papers by this authorCorresponding Author
Prof. Shivnath Mazumder
Department of Chemistry, Indian Institute of Technology Jammu, Jammu, 181221 India
Search for more papers by this authorCorresponding Author
Prof. Cláudio N. Verani
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
Search for more papers by this authorDr. Nour El Harakeh
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
These authors contributed equally to this work.
Search for more papers by this authorDr. Ana C. P. de Morais
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
These authors contributed equally to this work.
Search for more papers by this authorNeha Rani
Department of Chemistry, Indian Institute of Technology Jammu, Jammu, 181221 India
These authors contributed equally to this work.
Search for more papers by this authorDr. Javier A. G. Gomez
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
Search for more papers by this authorAbigail Cousino
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
Search for more papers by this authorCorresponding Author
Prof. Mauricio Lanznaster
Instituto de Química, Universidade Federal Fluminense, 24020-141 Niterói, RJ, Brazil
Search for more papers by this authorCorresponding Author
Prof. Shivnath Mazumder
Department of Chemistry, Indian Institute of Technology Jammu, Jammu, 181221 India
Search for more papers by this authorCorresponding Author
Prof. Cláudio N. Verani
Department of Chemistry, Wayne State University, Detroit, MI, 48202 USA
Search for more papers by this authorDedicated to Professor Phalguni Chaudhuri
Abstract
Two heterometallic photocatalysts were designed and probed for water reduction. Both [(bpy)2RuIINiII(L1)](ClO4)2 (1) and [(bpy)2RuIINiII(L2)2RuII(bpy)2](ClO4)2 (2) can generate the low-valent precursor involved in hydride formation prior to dihydrogen generation. However, while the bimetallic [RuIINiII] (1) requires the presence of an external photosensitizer to trigger catalytic activity, the trimetallic [RuIINiIIRuII] (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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