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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： Luo, Yixin 1 ; Ma, Ruitong 1 ; Sun, Chengjie 1 ; Yu, Tongyan 1 ; Yan, Haoxuan 1 ; Zhou, Xiaomei 1 ; Guan, Qingxin 1 ; Qiu, Mo 2 ; Li, Wei 1 ;

作者机构： 1.Nankai Univ, Coll Chem, State Key Lab Elemento Organ Chem, Key Lab Adv Energy Mat Chem,Minist Educ, Tianjin 300071, Peoples R China

2.Chinese Acad Agr Sci, Agroenvironm Protect Inst, 31 Fukang Rd, Tianjin 300191, Peoples R China

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

期刊名称：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY （ 影响因子：21.1； 五年影响因子：20.2 ）

ISSN： 0926-3373

年卷期： 2026 年 381 卷

页码：

收录情况： SCI

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 H delta+/H delta- species that synergistically promote cellulose hydrolysis and hydrogenation. Under optimized conditions (200 degrees 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 FLPsmediated 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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