Research at BioLEC

 

The chemical industry accounts for 10% of energy consumption globally, generating 7% of all greenhouse gas emissions in the manufacture of everyday chemicals and materials. BioLEC brings together a diverse group of researchers with the aim of using light to supercharge catalysts in the way that Nature harvests multiple photons to power reactions. This will enable photocatalysts to drive transformations more effectively and efficiently, thereby reducing this energy burden.

 

Research in the Center focuses on developing and improving light-powered catalysts and the reactions they facilitate to use in generating specific and valuable chemical products from more stable and abundant starting materials, such as waste matter like sawdust or plastic bags.

We advance towards this mission through research in three thrusts:

Thrust A: Innovate

To develop innovative photochemistry that enables new routes for synthesizing chemical feedstocks

Thrust B: Exploit

To discover, synthesize, and study photoenzymes that enable enhanced catalysis

Thrust C: Elucidate

To inform the design of new photocatalysts by elucidating photocatalysis mechanisms

Thrust A: Innovate

Overview

To develop innovative photochemistry that enables new routes for synthesizing chemical feedstocks

Research portfolio

Photochemistry, recycling, contrathermodynamic transformations

Focus: Develop novel tools to discover and control mechanisms for macromolecular transformations. Our studies of photo-catalyzed polymer decomposition, already demonstrated to work on a variety of systems, address this aim and will be developed and expanded further in the next cycle. To extend beyond one-photon redox processes we will develop multiple-photon absorbers to generate solvated electrons and super-oxidants.

Example publications

Kuo Zhao, Robert R. Knowles, “Contra-Thermodynamic Positional Isomerization of Olefins”, J. Am. Chem. Soc. 2022144, 137, available online

Suong T. Nguyen, Elizabeth A. McLoughlin, James H. Cox, Brett P. Fors, Robert R. Knowles, “Depolymerization of Hydroxylated Polymers via Light-Driven C-C Bond Cleavage”, J. Am. Chem. Soc. 2021143, 12268, available online and explanatory slide.

Robert Knowles

Robert Knowles

Thrust A leader

Professor of Chemistry

Princeton University

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Felix Castellano

Felix Castellano

Thrust A leader

Professor, Goodnight Innovation Distinguished Chair

North Carolina State University

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Thrust B: Exploit

Overview

To discover, synthesize, and study photoenzymes that enable enhanced catalysis

Research portfolio

Spectroscopy, biosynthesis, biocatalysis

Focus: BioLEC’s work on transforming enzyme’s catalytic abilities with light provides not only innovative functionality but also key insights into the fundamental functions of the microenvironment within the protein. Additionally, bio-inspired tactics from photocatalysis involve separating catalytic functions to improve efficiency or selectivity.

Example publications

Bryce Nicholls, Daniel Oblinsky, Sarah Kurtoic, Daria Grosheva, Yuxuan Ye, Gregory D. Scholes, Todd Hyster, “Engineering a Non-Natural Enzyme for Improved Photon Efficiency”, Angew. Chem. Int. Ed. 20222, e202113842, available online

Paul T. Cesana, Beryl X. Li, Samuel G. Shepard, Stephen I. Ting, Stephanie M. Hart, Courtney M. Olson, Jesus I. Martinez-Alvarado, Minjung Son, Talia J. Steiman, Felix N. Castellano, Abigail G. Doyle, David W. C. MacMillan, Gabriela S. Schlau-Cohen, “A biohybrid strategy for enabling photoredox catalysis with low-energy light”, Chem 20228, 174, available online.

Gabriela Schlau-Cohen

Gabriela Schlau-Cohen

Thrust B Leader

Associate Professor of Chemistry

Massachusetts Institute of Technology

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Todd Hyster

Todd Hyster

Thrust B leader

Associate Professor of Chemistry and Chemical Biology

Cornell University

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Thrust C: Elucidate

Overview

Emulate and exploit biological systems for new or improved syntheses

Research portfolio

Organic synthesis, inorganic catalysts, spectroscopy

Focus: BioLEC has a strong track record using ultrafast laser spectroscopy, spectroscopies using short pulses of fast electrons, and time-resolved dielectric loss spectroscopy to reveal mechanisms of photocatalyzed reactions. We will extend our toolset by adding time-resolved x-ray spectroscopy and theory capabilities.

Example publications

Stephen I. Ting, Wendy L. Williams, Abigail G. Doyle, “Oxidative Addition of Aryl Halides to a Ni(I)-Bipyridine Complex”, J. Am. Chem. Soc. 2022144, 5575, available online.

Justin D. Earley, Anna Zieleniewska, Hunter H. Ripberger, Nick Y. Shin, Megan S. Lazorski, Z. J. Mast, Hannah J. Sayre, James K. McCusker, Gregory D. Scholes, Robert R. Knowles, Obadiah G. Reid, Garry Rumbles, “Ion-pair reorganization regulates reactivity in photoredox catalysts”, Nature Chem. 2022available online.

Abigail Doyle

Abigail Doyle

Thrust C Leader

Saul Winstein Chair in Organic Chemistry

University of California, Los Angeles

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Hannah Sayre

Hannah Sayre

Thrust C leader

Assistant Professor Chemistry and Chemical Biology/Chemical Engineering

Northeastern University

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