Work

Unveiling the mechanism for selective cleavage of C-C bonds in sugar reactions on tungsten trioxide–based catalysts

Year: 2022

Type: article

Abstract: Conversion of naturally occurring sugars, the most abundant biomass resources on Earth, to fuels and chemicals provides a sustainable and carbon-neutral alternative to the current fossil resource–based processes. Tungsten-based catalysts (e.g., WO 3 ) are efficient for selectively cleaving C-C bonds of sugars to C 2,3 oxygenate intermediates (e.g., glycolaldehyde) that can serve as platform molecules with high viability and versatility in the synthesis of various chemicals. Such C-C bond cleavage follows a mechanism distinct from the classical retro-aldol condensation. Kinetic, isotope 13 C-labeling, and spectroscopic studies and theoretical calculations, reveal that the reaction proceeds via a surface tridentate complex as the critical intermediate on WO 3 , formed by chelating both α- and β-hydroxyls of sugars, together with the carbonyl group, with two adjacent tungsten atoms (W-O-W) contributing to the β-C-C bond cleavage. This mechanism provides insights into sugar chemistry and enables the rational design of catalytic sites and reaction pathways toward the efficient utilization of sugar-based feedstocks.

Source: Proceedings of the National Academy of Sciences

DOI: 10.1073/pnas.2206399119

Authors: Yue Liu, Wei Zhang, Cong Hao, Shuai Wang, Haichao Liu

Institutions: Peking University, Beijing National Laboratory for Molecular Sciences, Xiamen University, Collaborative Innovation Center of Chemistry for Energy Materials

Language: English

Topic: Catalysis for Biomass Conversion

Subfield: Biomedical Engineering

Field: Engineering

Domain: Physical Sciences

Open Access status: hybrid

Funders: National Natural Science Foundation of China, Institute of Chemistry, Chinese Academy of Sciences, National Key Research and Development Program of China, Beijing National Laboratory for Molecular Sciences