Supramolecular Materials Chemistry

Our research program exists at the interface of synthetic chemistry and materials science, addressing fundamental scientific challenges related to supramolecular assembly, functional materials, and environmental sustainability. Our group leverages expertise in non-covalent interactions and dimensional order in the development of chemical tools for the by-design construction and programmed destruction of functional materials. Students in our group will receive extensive training in synthetic organic and inorganic chemistry, through the design and preparation of organic building blocks and hybrid organic–inorganic materials, and in analytical tools, through characterizing these materials using various techniques, including spectroscopy, adsorption measurements, and X-ray crystallography.

Stimulus-Responsive Frameworks

As we shift towards more energetically sustainable technologies, the development of advanced porous adsorbents for small molecule storage, carrier, and separation applications is necessary. Permanently porous coordination frameworks, namely metal–organic frameworks, have been widely pursued in this vein. Yet owing to the structurally rigid nature of most frameworks, their performance in processes requiring successive cycles of adsorption–desorption are inefficient and energy consumptive.  Alternatively, porous frameworks that alter their structure and porosity in response to external stimuli, such as pressure and temperature, may serve to improve the performance efficiency in such processes. Our efforts will seek to develop stimulus-responsive frameworks for specific applications relevant to the sustainable energy future. 

Chemical Recycling of Polyolefins 

Polyolefinic plastic waste has become an environmental crisis due to ubiquitous use, poor biodegradability, and negligible mechanical recycling. To mitigate this growing waste stream, energy-efficient chemical recycling processes, which selectively yield valuable small molecules must be sought. Unfortunately, the controlled depolymerization of polyolefins remains poorly understood. To advance the fundamental understanding of these chemical events and elucidate catalyst design principles, our group will synthesize and study heterogeneous catalysts with spatially defined local environments capable of controllably depolymerizing polyolefins under mild thermal conditions. The success of these efforts will advance mechanistic insight into hydrocarbon scission and confinement effects, and, we hope, ultimately help lead to the remediation of plastic pollution.

Check out the video we made with the Trefny Teaching Center on campus to introduce our research to general chemistry students at Mines.

Non-Covalently Linked Porous Materials

The properties and utility of synthetic permanently porous frameworks are largely determined by the mode of intermolecular connectivity. As such, constructing porous framework materials through unconventional intermolecular interactions can help meet the requirements of emergent applications in catalysis, gas capture, molecular separations, and energy harvesting and storage. Our group will seek to realize  new families of permanently porous organic frameworks, in which the crystalline order of molecular building blocks is constructed through directional non-covalent interactions. Our efforts will undertake a multi-pronged approach to tecton and framework design, with the ultimate goal of establishing non-covalent interactions as a ubiquitous tool in porous framework assembly through the development of generalizable methodologies for the synthesis of robust, modular, and functional frameworks.

Unnatural DNA Base Pairs

Hydrogen bond (HB)-driven base pairing between A–T and G–C is the means through which genetic information is stored, translated, and passed down through generations. Therefore, the discovery of synthetic nucleotides that form unnatural base pairs through alternative non-covalent attractions would expand the genetic alphabet, dramatically increasing information storage and function in DNA. Through this work our group seeks to establish emergent non-covalent interactions as a modular and predictable tool for unnatural base pairing, with the ultimate goal of achieving a new class of high-fidelity base pairs compatible with endogenous cellular machinery. The development of new base pairs will influence many aspects of DNA-based technologies, including nanomaterials assembly, detection and therapy, and achieving form and function in semi-synthetic organisms. Moreover, this work will yield a greater fundamental comprehension of poorly understood non-covalent  interactions.

© 2019