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Few aspects are as prevalent and important to energy conversion and storage as the dimension control of porous nanomaterial architectures. Electrochemical reactions all depend significantly on the dimensions and pathway connectivity of each transport process (red, ox, e-) where both the material walls and the pores each control distinct processes. Despite the fundamental importance of nanoscale architecture, the study of these processes is limited by a lack of well-defined architectures with independent control of pore and wall dimensions. Measurement of architecture-dependent properties requires architecture series with constant morphology (isomorphic) to eliminate the effects of varying pathway connectivity. In my talk, I will focus on recent developments with a new nanofabrication tool kit based upon the kinetic entrapment of block copolymer templates. Kinetic control is historically difficult to reproduce, a challenge that we have resolved with switchable micelle entrapment to yield reproducible and homogeneous nanomaterial series that follow model predictions. This approach enables seamless access from meso-to-macroporous materials with unprecedented ~2 Å precision of tuning, commensurate with the underlying atomic dimensions. This precision and independent control of architectures also opens new opportunities to broadly realize nano-optimized devices.
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