数字农科院2.0

P-modulated NiP active centers and PNC support enabling synergistic H2/H2O activation in cellulose cascade conversion

文献类型： 外文期刊

作者： Yixin Luo;Ruitong Ma;Chengjie Sun;Tongyan Yu;Haoxuan Yan;Xiaomei Zhou;Qingxin Guan;Mo Qiu;Wei Li

作者机构：

关键词： Activated H2 heterolysis;Bifunctional catalyst;Biomass conversion;Frustrated Lewis pars;Hydrolysis of cellulose

期刊名称： Applied Catalysis B: Environmental

ISSN： 0926-3373

年卷期： 2025 年 381 卷

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： The catalytic valorization of cellulose into sorbitol offers a sustainable pathway for biomass resource utilization, yet its efficiency remains constrained by suboptimal synergy between hydrolysis and hydrogenation processes. Herein, an innovative strategy was proposed for constructing a phosphorus/nitrogen co-doped carbon layer supported nickel phosphide catalyst (NiP/PNC) via coordination-driven self-assembly. The engineered P/N co-doped carbon layer creates an electron-rich microenvironment, significantly enhancing H+ generation through efficient H2O adsorption and polarization. Meanwhile, frustrated Lewis pairs (FPLs) formed at the NiP-OH interface drive heterolytic H2 dissociation, yielding highly reactive Hδ+/Hδ− species that synergistically promote cellulose hydrolysis and hydrogenation. Under optimized conditions (200 °C, 5 h, 4 MPa H2), the NiP/PNC catalyst achieved a remarkable sorbitol yield exceeding 90 % in water and demonstrated satisfactory cyclic stability. Experimental characterizations and DFT calculations reveal that the bifunctional active sites coordinate a cascade reaction pathway: the electron-deficient P/N-doped carbon facilitates H2O activation, while FLPs-mediated H2 heterolysis substantially reduces the energy barrier for hydrogen dissociation. This work pioneers a catalysis modulation strategy through rational electronic and structural modulation, providing fundamental insights into the design of multifunctional catalysts for sustainable biomass conversion.

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