.png){kind=icon}
.png){kind=icon}
Return
High-Efficiency Dual-Site Biomimetic Catalyst for Lignin Depolymerization
.png){kind=icon}
PRE
AI
DOI：10.1021/acscatal.4c07113.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
Developing biomimetic catalysts with enhanced catalytic efficiency is a promising strategy to address the challenges of lignin depolymerization under mild conditions. In this study, we designed a dual-site biomimetic catalyst, Pd@Ce-PZDC, engineered to emulate the lignin-degrading functions of natural laccase and peroxidase enzymes, thereby facilitated lignin depolymerization. The laccase-like activity of Pd@Ce-PZDC exhibited a catalytic efficiency (V max/K m) of 1.3 x 10-2 min-1, which is 3.14 times higher than that of natural laccase and 1.62 times greater than that of the single-site bioinspired laccase MOF catalyst Ce-PZDC. Its peroxidase-like activity, assessed with TMB and H2O2, is 5.6 and 11.2 times higher, respectively, than that of Ce-PZDC. Density Functional Theory (DFT) calculations indicated a synergistic dual-site effect where Pd NPs activate Ce(IV) within the MOF, imparting it with laccase-like activity akin to Ce(III), thereby increasing the number of active sites and enhancing overall catalytic efficiency. Under mild conditions (60 degrees C in aqueous solution), Pd@Ce-PZDC demonstrated high efficiency in the oxidative depolymerization of birch lignin, selectively cleaving beta-O-4 and beta-beta linkages. This resulted in a reduction in molecular weight of lignin and produced aromatic monomers (approximately 13.0%), including vanillin, syringaldehyde, and vanillic acid. This dual-site synergistic strategy offers a promising avenue for valorization of lignin and the development of effective catalytic systems for biomass conversion.
Keywords:
biomimetic catalysis
lignin depolymerization
metal-organic frameworks
palladium nanoparticles
synergistic catalysis
Journal
IF:
13.1
Papers:
1.6W
Citations:
15.0W
Organization
No organization information available