祝贺孙成杰的论文发表在ACS Appl. Mater. Inter.
Interfacial Engineering of Frustrated Lewis Pairs for Promoting Cellulose-to-Sorbitol Cascade Conversion
Chengjie Sun, Yixin Luo, Mo Qiu,* Qingxin Guan,* Ruitong Ma, Zilu Zhang, Feng Shen, Shizhou Shen, Jirui Yang, and Wei Li*, ACS Appl. Mater. Inter., 2026, 18, 37691-37702.
https://doi.org/10.1021/acsami.6c06071
Abstract：
Insufficient synergy between hydrolysis and hydrogenation seriously hinders the efficient conversion of insoluble cellulose in biomass utilization. Herein, using tobacco straw-derived lignin to prepare ordered mesoporous carbon (OMC), we report a complex-mediated strategy for constructing a Ni–P–O@NixP/OMC catalyst with tailored P–C–O doped sites and Niδ+–P–Oδ− frustrated Lewis pairs (FLPs). Characterizations and DFT results indicate that the P–C–O sites in a P/O-doped OMC support promote H2O adsorption and polarization, accelerating H3O+ generation for enhanced cellulose hydrolysis. Simultaneously, the Niδ+–P–Oδ− FLPs on the NixP surface promote H2 heterolysis and H2O dissociation, generating highly active Hδ+/Hδ– and H3O+ species that synergistically enhance hydrolysis and hydrogenation. Benefiting from the spatial coupling of hydrolysis and hydrogenation at the atomic scale, the prepared catalyst achieves an 80% sorbitol yield from cellulose in water at a low Ni loading of 4.5 wt %, along with satisfactory cycling stability. Increasing the Ni content to 8.0 wt % further raises the sorbitol yield to 89.5%, outperforming most reported noble-metal-based catalysts. Finally, a sorbitol yield in excess of 90% is obtained by using the residue after lignin extraction as the substrate. This work establishes a design paradigm for efficient cascade biomass conversion by creating atomic-scale P–C–O sites and Niδ+–P–Oδ− FLPs that enable spatially coupled hydrolysis and hydrogenation through tailored electronic structures.
