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The
U.S. and the World face an urgent challenge: to transform the way we
power and fuel our economy. Developing cost-effective alternative
energy sources to meet current and future energy demand in an
environmentally responsible manner is critical to achieve both energy
security and overall sustainability. These challenges require an
unprecedented response, and call for the development of
interdisciplinary research and educational programs integrating
expertise that transcends traditional disciplinary boundaries.
The
Yale Energy initiative aims to demonstrate the feasibility of using
oxomanganese catalysts immobilized on TiO2
nanoparticles (NPs) to achieve photocatalytic water oxidation. The team
is integrated by 4 co-PI’s, including Batista,
Brudvig, Crabtree and Schmuttenmaer,
and is currently funded by the grant DE-FG02-07ER15909 from the Office
of Basic Energy Sciences, Office of Science, U.S. Department of Energy
(DOE). We also have a generous allocation of DOE supercomputer time
from NERSC.
We
offer our trainees, including students and post-docs, an opportunity to
work with multiple PI’s and gain interdisciplinary research training in
synthesis and characterization of our own catalytic surface complexes;
computational modeling of both structure and dynamics; femtosecond
spectroscopy for probing ultrafast interfacial processes; and
quantitative electrochemical studies of oxidation chemistry, as coupled
to fuel production. Crabtree
contributes expertise in inorganic chemistry, with particular reference
to oxidation chemistry using oxo-Mn complexes and the design and
synthesis of robust ligands for catalysis; Brudvig has
extensive experience in structural and mechanistic studies of
biomimetic complexes for O2
evolution and oxygenation of saturated CH bonds, including
characterization via EPR spectroscopy and electrochemical methods; Schmuttenmaer
provides expertise in laser spectroscopy applied to studies of
interfacial electron transfer (IET), having pioneered the field of
time-resolved THz spectroscopy as a non-contact electrical probe with
sub-picosecond time resolution; and Batista
complements all the experimental work with theoretical studies of
chemical dynamics and electronic structure calculations relevant to
water-splitting catalysts and IET in functionalized TiO2.
Our
mission is to impart to our trainees the intellectual and practical
skills needed to address the urgent energy challenges of the
twenty-first century, gaining experience relevant to both academic and
nonacademic careers and engaging in strong collaborations with national
laboratories and industries early in their research careers. We aspire
to succeed in producing researchers with training in the emerging
fields of chemistry related to the sustainable production of chemical
fuels, and in the fundamentals on which they are grounded, with an
international perspective who will push at the frontiers of
interdisciplinary programs in alternative energy and become future
leaders of the field.
Recent
Publications
9. Energy & Environ. Sci.
(2008) (in revision) Deposition of an oxomanganese water oxidation
catalyst on TiO2
nanoparticles; computational modeling, assembly and characterization.
G. Li, E.
M. Sproviero, R. C. Snoeberger III, N.
Iguchi,
J. D. Blakemore, R.
H. Crabtree, G. W. Brudvig, and V. S. Batista.
8. Proc. SPIE (2008)
7034:
70340C 1-8. Characterization of Siloxane
adsorbates covalently attached to TiO2. N.
Iguchi,
C. Cady, R.
C. Snoeberger III, B. M. Hunter, E. M. Sproviero, C. A. Schmuttenmaer,
R. H. Crabtree, G. W. Brudvig, and V. S. Batista.
7. J. Am. Chem. Soc. (2008)
130: 14329-14338. Acetylacetonate anchors for robust
functionization of TiO2
nanoparticles with Mn(II)-terpyridine
complexes. W. R. McNamara, R. C. Snoeberger III, G. Li, J. M.
Schleicher, C. W. Cady, M. Poyatos, C. A. Schmuttenmaer, R. H.
Crabtree, G. W. Brudvig, and V. S. Batista.
6. J. Am. Chem. Soc. (2008)
130: 6728-6730. A model of the oxygen evolving center
of photosystem II
predicted by structural refinement based on EXAFS simulations. E. M.
Sproviero, J. P. McEvoy, J. A. Gascon, G. W. Brudvig, and V. S.
Batista.
5. J. Phys. Chem. B. (2007)
111: 11982-11990. Ultrafast photooxidation of a Mn(II)-terpyridine
complex covalently attached to TiO2
nanoparticles. S. G. Abuabara, C. W. Cady, J. B. Baxter, C. A.
Schmutternmaer, R. H. Crabtree, G. W. Brudvig and V. S. Batista.
4. Science (2006)
312:
1941-1943.
Molecular recognition in the selective oxygenation of saturated
C-H
bonds by adimanganese catalyst. Das, S., C.D. Incarvito, R.H. Crabtree,
and G.W. Brudvig.
3. J. Am. Chem. Soc. (2003)
125: 7889-7997. Quantum dynamics simulations of
interfacial electro transfer in sensitized TiO2
semiconductors. Rego, L.G.C. and V.S. Batista.
2. J. Phys. Chem. B. (2002)
106: 7146-7159. Terahertz spectroscopy. Beard, M.C., G.M.
Turner, and C.A. Schmuttenmaer.
1. Science (1999)
283: 1524-1527. A functional model for O-O bond
formation by the O2-evolving
complex in photosystem II. Limburg, J. , J.S. Vrettos, L.M.
Liable-Sands, A.L. Rheingold, R.H. Crabtree, and G.W. Brudvig.
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