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Abstract:

A major focus of green and sustainable chemistry research has been to try to find ways to produce the same chemicals we use today from sustainable sources. Such a challenge usually involves the deconstruction and major modification of biomass’s three constituent polymers: cellulose and hemicellulose, which are both polysaccharides; and lignin, which is a polymer of phenyl propanoid sub-units. If these three polymers can be broken down into sugars or lignin monomers, multi-step biological and catalytic processes are then required to produce molecules identical to those currently derived from petroleum. In both depolymerization and catalytic upgrading, the biggest challenge is not achieving the desired reaction, but rather avoiding being outcompeted by other, detrimental reactions, such as degradation reactions, side reactions, or catalyst deactivation. These issues, along with the complexity of transforming natural structures to petroleum structures, has plagued the development of biobased chemicals.

In this talk, I will present several approaches to these challenges that my lab has developed, which notably preserve and build on these natural structures, rather than transforming them into petroleum-like replacements. I will show how we can use functionalization chemistry, both during lignin extraction and polysaccharide depolymerization, to reversibly ‘trap’ stabilized intermediate molecules, preserve their structure, and facilitate their high-yield upgrading^1,2. I will also discuss how targeted surface modifications on the heterogeneous catalysts associated with these transformations can lead to dramatic changes in activity, stability and selectivity, even in the presence of highly oxygenated renewable streams^3,4. Finally, I will discuss how this same functionalization can be used to create new commodity chemicals, including polymers, that build new products around these preserved natural structures, as opposed to trying to replicate petroleum structures^5,6. I will discuss how the presence of these natural structures leads to molecules that are, by their very design, much easier to produce and more sustainable than current alternatives.

References:

1 L. Shuai, M. T. Amiri, Y. M. Questell-Santiago, F. Héroguel, Y. Li, H. Kim, R. Meilan, C. Chapple, J. Ralph and J. S. Luterbacher, Science, 2016, 354, 329–333.

2 Y. M. Questell-Santiago, R. Zambrano-Varela, M. T. Amiri and J. S. Luterbacher, Nat. Chem., 2018, 1222–1228.

3 J. H. Yeap, F. Héroguel, R. L. Shahab, B. Rozmysłowicz, M. H. Studer and J. S. Luterbacher, ACS Catal., 2018, 8, 10769–10773.

4 B. P. Le Monnier, F. Wells, F. Talebkeikhah and J. S. Luterbacher, Adv. Mater., 2019, 31, 1904276.

5 A. O. Komarova, G. R. Dick and J. S. Luterbacher, Green Chem., 2021, 23, 4790–4799.

6 L. P. Manker, G. R. Dick, A. Demongeot, M. A. Hedou, C. Rayroud, T. Rambert, M. J. Jones, I. Sulaeva, M. Vieli, Y. Leterrier, A. Potthast, F. Maréchal, V. Michaud, H.-A. Klok and J. S. Luterbacher, Nat. Chem., 2022, 1–9.

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Bio:

Jeremy Luterbacher was born in Switzerland in 1984 and received a B.Sc and M.Sc. in chemical engineering from the École Polytechnique Fédérale in Lausanne (EPFL), Switzerland in 2007. He spent a year as a visiting scientist at the Massachusetts Institute of Technology (MIT) working in Jeff Tester’s lab. Jeremy then moved to Cornell University in Ithaca, New York, to pursue doctoral studies in Prof. Larry Walker’s lab. After receiving his PhD in 2012, Jeremy joined the Great Lakes Bioenergy Research Center at the University of Wisconsin-Madison as a Swiss National Science Foundation Postdoctoral Scholar under the supervision of Prof. Jim Dumesic. In 2014, Jeremy returned to EPFL as a Tenure-Track Assistant Professor and head of the Laboratory of Sustainable and Catalytic Processing. He was promoted to Associate Professor in 2021.

Since arriving at EPFL, Jeremy has been awarded a European Research Council (ERC) starting grant in 2017 and a Swiss National Science Foundation Consolidator Grant in 2023. In 2019, he received the Werner Prize from the Swiss Chemical Society for outstanding independent chemical research in Switzerland. His work on lignin stabilization was recognized by the 2019 EPFL Latsis prize and the 2021 ACS Sustainable Chemistry & Engineering Lectureship. He is also an associate editor at Science Advances.