Porous hollow nanospheres nickel phosphide and its high catalytic hydrogenation performance on naomaohu coal soluble portion and model compounds

• Published in: Fuel (Guildford) 2024-08, Vol.370, p.131774, Article 131774
• Main Authors: Zhang, Yingxiong, Liu, Ting, Tang, Yakun, Liu, Jingmei, Zhang, Yue, Zhou, Xiaodong, Li, Xiaohui, Liu, Lang
• Format: Article
• Language: English
• Subjects: Catalytic hydroconversion; Coal soluble portion; Hollow nanosphere nickel phosphide; Oxygen-containing compounds
• ISSN: 0016-2361; 1873-7153
• DOI: 10.1016/j.fuel.2024.131774

A hollow nanosphere Ni3P catalyst was prepared via a simple phase separation method. The hollow structure was conducive to exposure of the catalytic site, and the electron-rich nickel exhibited a good catalytic activity. During the reaction at 140℃ and 1.0 MPa for 2h, the conversion rate of benzyl phenyl ether (BPE) was 100%. For the naomaohu coal (NMHC) soluble portion, it has good catalytic hydrogenation and deoxygenation performance, with an increase in alkane content from 19% to 47% and a decrease in oxygen-containing compounds from 56% to 21%. [Display omitted] •The Ni3P catalyst with hollow nanosphere structure showed good catalytic activity.•H radical and diatomic hydrogen are the main active hydrogen species for the catalytic hydroconversion.•Ni3P can effectively promote C-O bond fracture in soluble portion.•The oxygen compounds in soluble portion decreased from 56% to 21%. The catalytic conversion of oxygen-containing aromatic ring in lignite under mild conditions is crucial to obtain clean liquid fuel. Here, hollow nanosphere Ni3P-500–24 catalysts were prepared at a calcination temperature of 500 °C and acid-etching time of 24 h. The porous hollow nanospheres structure could expose more catalytic sites, and the electron-rich nickel exhibited a good catalytic activity. The conversion rate of benzyl phenyl ether (BPE) was 100 % (140 ℃, 1 MPa H2, 2 h), and the main products were methylcyclohexane and cyclohexanol, indicating that the catalyst had good catalytic hydrocracking performance. In addition, the catalyst exhibited certain deoxygenation activity and high product selectivity for other oxygen-containing model compounds. For the catalytic hydrogenation of Naomaohu coal (NMHC) soluble portion, the content of alkanes increased from 19 % to 47 %, while the content of oxygen-containing compounds decreased from 56 % to 21 %, which further demonstrate that the catalyst have good catalytic hydrogenation and deoxygenation performance. Density Functional Theory (DFT) calculations showed that the properties of the Ni3P-500–24 catalyst was similar to noble metal, which could activate H2 to produce two kind of active hydrogen: H radical and diatomic hydrogen. The synergistic pathways for the transfer of active hydrogen during the catalytic hydroconversion (CHC) process were analyzed. Above results could provide theoretical guidance for the conversion of lignite into high-quality clean liquid fuels.