FY2010 - Oak Ridge National Laboratory

Director’s R&D Fund—
Science for Extreme Environment: Advanced Materials and Interfacial Processes for Energy
orthogonal linking reaction; (3) synthesis of a library of functional polymers suitable for attachment to the
central core; (4) characterization of a series of centro-symmetric star copolymers by light scattering; and
(5) production of model three-arm stars by sequential orthogonal attachment of different arms. In
addition, efforts have been made to test and optimize conditions of attachment using “clickable” base
layers grafted to surfaces. In total this project has led to enhanced capabilities in characterization of soft
materials using light scattering methods and also fostered new synthetic routes for making complex
copolymers. These accomplishments and capabilities have recently attracted new users to the Center for
Nanophase Materials Sciences. In addition, the vein of research nucleated through this project will
continue through programmatic efforts aimed at investigating how chemical information and interactions
integrated into the macromolecules affect their assembly at surfaces and in solution, as well as their
nanoscale structure and dynamics.
Information Shared
He, L., J. P. Hinestrosa, J. M. Pickel, S. Zhang, D. G. Bucknall, S. M. Kilbey, J. W. Mays, and K. Hong.
2011. “Fluorine-Containing ABC Linear Triblock Copolymers: Synthesis and Self-assembly in
Solutions.” J. Poly. Sci.: Part A.: Polym. Chem. 49, 414–422. Published online on Nov. 23, 2010.
05375
Attoliter Droplets on Demand in Nanochannels: New Opportunities
for Investigating Chemical Reactivity and Catalysis
in Nanoscale Reactors
Seung-Yong Jung, Scott Retterer, and Charles Patrick Collier
Project Description
We propose a new method for producing submicron, attoliter-scale (10 -17 L) aqueous droplets on demand
at the intersection of nanochannels. At the intersection of two apposed aqueous channels with an
immiscible oil channel, two submicron, oil-dispersed aqueous droplets containing different reactants can
be forced to collide with each other and fuse, completely mixing their interior contents by diffusion in less
than a millisecond. This can be used to produce monodisperse reaction vessels two orders of magnitude or
smaller in volume than in current state-of-the-art microfluidic devices, while satisfying the constraints of
perfect sealing and passivation against nonspecific adsorption of large macromolecules like proteins at the
droplet periphery. The resulting surface-to-volume (S/V) ratios of droplets at this scale will be in excess
of 10 6 , which may open up new areas of research across several fronts, in particular the study of catalysis
and reaction dynamics of transient chemical and biochemical intermediates in confined environments. As
a proof-of-principle demonstration of the method, we will measure single-enzyme kinetics in the
nanoreactors with a well-defined time zero for initiating the reaction, and with sub-millisecond temporal
resolution.
Mission Relevance
The ability to probe reaction dynamics of highly reactive, transient chemical, biochemical, and
electrochemical species in confined environments with unprecedented temporal resolution will provide
important new capabilities vital to next-generation DOE missions. Results from this work will add to our
fundamental understanding of catalysis, chemical synthesis, and energy in nanoscale confined systems,
and thus may be directly applicable to targeted DOE initiatives such as advanced materials, advanced
energy systems, and systems biology. In addition, practical technological advances, such as in sensors and
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