Biomass deconstruction and chemical functionalization
Biomass deconstruction aims to depolymerize the major plant biopolymers such as cellulose, hemicellulose (i.e. polysaccharides) and lignin (a heteropolymer of phenylpropanoid subunits). Lignin is especially easily destroyed during pulp and paper processing and most biorefinery processes. Our group is developing chemical functionalization techniques to avoid lignin destruction during extraction and to produce unique functionlized platform from both lignin and carbohydrates. Through functionalization, we notably aim to directly produce useful products during deconstruction. We also use fractionation to answer fundamental questions about lignin structure and chemistry.
Researchers involved in this work: Stefania Bertella, Songlan Sun, Claire Bourmaud, and Jean Behaghel
Recent work:
S. Bertella and J. S. Luterbacher*. “Simultaneous extraction and controlled chemical functionalization of hardwood lignin for improved phenolation”. Green Chemistry, 23, 3459–3467, 2021. doi:10.1039/D1GC00358E
J. Behaghel de Bueren, F. Héroguel, C. Wegmann, G. R. Dick, R. Buser and J. S. Luterbacher*. “Aldehyde-Assisted Fractionation Enhances Lignin Valorization in Endocarp Waste Biomass”. ACS Sustainable Chemistry & Engineering, 8, pp. 16737–16745, 2020. doi: 10.1021/acssuschemeng.0c03360
M. Talebi Amiri, G. R. Dick, Y. M. Questell-Santiago, and J. S. Luterbacher*. “Fractionation of lignocellulosic biomass to produce uncondensed aldehyde-stabilized lignin”. Nat. Protoc., 14: pp. 921-954, 2019. doi: 10.1038/s41596-018-0121-7
Y. M. Questell-Santiago, R. Zambrano-Varela, M. Talebi Amiri, and J. S. Luterbacher*. “Carbohydrate stabilization extends the kinetic limits of chemical polysaccharide depolymerization”. Nat. Chem., 10: pp. 1222-1228, 2018. doi: 10.1038/s41557-018-0134-4
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*. “Formaldehyde stabilization facilitates lignin monomer production during biomass depolymerization”. Science, 354 (6310): pp. 329-333, 2016. doi: 10.1126/science.aaf7810
Catalyst synthesis for renewable molecule production
Renewable biomass-derived molecules, unlike those produced from petroleum are highly oxygenated, and often produced in dilute-aqueous streams. Heterogeneous catalysts – the workhorses of the petrochemical industry – are sensitive to water and contain many metals that easily sinter and leach in liquid-phase conditions. The production of renewable chemicals from biomass, especially valuable aromatics, often requires expensive platinum group metals and suffers from low selectivity. New synthetic methods based on atomically precise metal oxide deposition could lead to solutions to these issues. At LPDC, we are working on synthesis methods to precisely control surface functionalities of heterogeneous catalysts through the atomically-precise deposition of highly tailored metal oxides. Initial work show that metal oxide coatings can eliminate irreversible deactivation of catalysts used in liquid phase conditions. In parallel, we can create multi-metal oxide clusters with near-atomic precision that can greatly increase activity and selectivity compared to conventional catalysts.
Researchers involved in this work: Farzaneh Talebkeikhah, Yu-Cheng Lin, Dr. Seongmin Jin, and Zezhong Li.
Recent work:
Y.-P. Du, A. M. Bahmanpour, L. Milošević, F. Héroguel, M. D. Mensi, O. Kröcher and J. S. Luterbacher*. “Engineering the ZrO2–Pd Interface for Selective CO2 Hydrogenation by Overcoating an Atomically Dispersed Pd Precatalyst”. ACS Catalysis, 10, 12058–12070, 2020. doi: 10.1021/acscatal.0c02146
B. P. Le Monnier, F. Wells, F. Talebkeikhah and J. S. Luterbacher*. “Atomic Layer Deposition on Dispersed Materials in Liquid Phase by Stoichiometrically Limited Injections”. Advanced Materials, 31, 1970373, 2019. doi: 10.1002/adma.201904276
Y-P. Du, F. Héroguel, and J. S. Luterbacher*. “Slowing the Kinetics of Alumina Sol-Gel Chemistry for Controlled Catalyst Overcoating and Improved Catalyst Stability and Selectivity”. Small, 14 (34): pp. 1801733, 2018. doi: 10.1002/smll.201801733
F. Héroguel, L. Silvioli, Y.-P. Du and J. S. Luterbacher*. “Controlled deposition of titanium oxide overcoats by non-hydrolytic sol gel for improved catalyst selectivity and stability”. J. Catal., 358: pp. 50–61, 2018. doi: 10.1016/j.jcat.2017.11.023
F. Héroguel, B. P. Le Monnier, K. S. Brown, J. C. Siu, and J. S. Luterbacher. “Catalyst stabilization by stoichiometrically limited layer-by-layer overcoating in liquid media”. Appl. Catal., B, 218: pp. 643–649, 2017. doi: 10.1016/j.apcatb.2017.07.006
Biobased product design
As we search for alternatives to fossil resources, biomass is an attractive sustainable feedstock especially for chemicals, which often need to be produced from complex carbon structures. However, producing direct drop-in replacements for petroleum from plants often involves too many transformations to be economical or sustainable. We use functionalization chemistry to create new products that are built around unmodified plant structures so as to be drastically easier to produce from biomass. This area spans all the way from new molecule synthesis and polymerization chemistry to material processing and characterization.
Researchers involved in this work: Lorenz Manker, Anastasiia Komarova, Songlan Sun, Luka Milosevic, Jean Behaghel, Maxime Hedou
Recent work:
L. P. Manker, G. R. Dick, A. Demongeot, M. A. Hédou, C. Rayroud, T. Rambert, M. J. Jones, I. Sulaeva, M. Vieli, Y. Leterrier, A. Potthast, F. Maréchal, V. Michaud, H.-A. Klok, J. S. Luterbacher*. “Sustainable polyesters via direct functionalization of lignocellulosic sugars” Nat. Chemistry, 14, 976–984, 2022. doi: 10.1038/s41557-022-00974-5
A. O. Komarova, G. R. Dick and J. S. Luterbacher*. “Diformylxylose as a new polar aprotic solvent produced from renewable biomass”. Green Chemistry, 2021. doi: 10.1039/D1GC00641JY. M. Questell-Santiago, J. H. Yeap, M. Talebi Amiri, B. P. Le Monnier and J. S. Luterbacher*. “Catalyst Evolution Enhances Production of Xylitol from Acetal-Stabilized Xylose”. ACS Sustainable Chemistry & Engineering, 8, 1709–1714, 2020. doi: 10.1021/acssuschemeng.9b06456
J. H. Yeap, F. Héroguel, R. L. Shahab, B. Rozmyslowicz, M. H. Studer, and J. S. Luterbacher*. “Selectivity control during the single-step conversion of aliphatic carboxylic acids to linear olefins”. ACS Catal., 8 (11): pp. 10769-10773, 2018. doi: 10.1021/acscatal.8b03370
F. Héroguel, B. Rozmysowicz, and J. S. Luterbacher*. “Improving Heterogeneous Catalyst Stability for Liquid-phase Biomass Conversion and Reforming”. Chimia, 69 (10): pp. 582–591, 2015. doi: 10.2533/chimia.2015.582