Abstract
Enhancing carbon utilization in biomass conversion makes a big challenge on sustainability. Herein, a novel catalytic system, MgO-D-lactic acid (D-LaA) was adopted, and a new “oligomer-first mechanism” was discovered for xylose transformation to a mixture very rich in D-LaA in a unique way. Supported by 13C NMR and DFT calculation, it was discovered that xylose oligomerized to C10/C15 through coupling of C–C bond via aldol condensation catalyzed by MgO species. The resultant oligomers were further split into C3 intermediates via selective C–C cleavage by Mg(OH)(H2O)3+ catalytic species. Besides, MgO-D-LaA catalytic system could also enable the reutilization of C2 by-product, glycolaldehyde, which was oligomerized to C4/C6 and further contributed to LaA production. These two factors synergistically made a significant breakthrough on carbon utilization for hemicellulose valorization, enabling the outstanding LaA yield up to 70.2 C-mol% with 73.1% ee value for D-LaA. The proposed oligomer mechanism comprehensively explained the origin of “excess” LaA yield beyond 60% via the conventional “3 + 2” pathway. This work made a significant breakthrough for the improvement of carbon utilization in xylose transformation to LaA, and allowed for the sufficient use of carbon atoms in xylose.
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