Global concerns regarding the economy, environment and sustainable energy resources dictate an urgent need for the design of novel catalytic reactions. We have recently discovered novel, environmentally benign reactions catalyzed by pincer complexes, including an entirely new reaction, namely the direct coupling of alcohols with amines to produce amides and H2 (Science, 2007, 317, 790). We believe that the mechanisms of these reactions involve a new concept in catalysis: metal-ligand cooperation by aromatization-dearomatization of the ligand. Such cooperation can play key roles also in the activation of H2, C-H, and other bonds. Remarkably, we have very recently discovered a new strategy towards light-induced water splitting into H2 and O2, also based on metal-ligand cooperation in a pincer system, and have observed an unprecedented O-O bond formation process (Science, in press). The design of efficient catalytic systems for splitting water into hydrogen and oxygen, driven by sunlight, and without use of sacrificial reagents, is among the most important challenges facing science today, underpinning the potential of hydrogen as a clean, sustainable fuel. In this context, it is essential to enhance our understanding of the fundamental chemical steps involved in such processes. We plan to (a) explore the scope of bond activation and catalysis based on the new concept of metal ligand cooperation by aromatization-dearomatization (b) study the mechanism and scope of the newly discovered novel approach towards water splitting by light (c) develop novel environmentally benign catalytic reactions involving O-H, C-H and other bonds, such as anti-Markovnikov hydration of alkenes (d) develop unprecedented asymmetric catalysis using chiral cooperating ligands (e) develop new CO2 chemistry, including its hydrogenation to methanol and photolytic splitting to CO and O2. The research is expected to lead to novel catalysis, of importance to environment and sustainable energy.
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