Lignin obtained from lignocellulosic biomass is an abundant, renewable, low-cost resource whose carbon-rich, aromatic composition makes it ideal to displace some petroleum-based feedstocks as chemical precursors. This project addresses challenges presented by the selective catalytic deconstruction of lignin to aromatic monomers, specifically by elucidating reactions and mechanisms involved in the disassembly of lignin using in-situ magic-angle-spinning (MAS) solid-state nuclear magnetic resonance (NMR) and high-resolution mass spectrometry (HR-MS). Cu-based catalysts supported on various materials (i.e., porous metal oxide and alumina) in different alcohol solvents can effectively depolymerize lignin, or even biomass, to generate aromatic-rich organic liquids with little or no coke and char formation. Our research will apply the unique capabilities and expertise at Environmental Molecular Science Laboratory (EMSL) of the Pacific Northwest National Laboratory (PNNL) to investigate the roles 1) catalysts composition (i.e., metal loading and support type), 2) solvent (e.g., methanol and 2-propanol), and 3) temperature/time profile play in lignin disassembly, rates of disassembly, and product distributions generated. The results of this Science Theme research will allow us to understand and establish the fundamental relationships that control solvo-catalytic disassembly of lignin and determine the resulting aromatic product yield and distribution.