期刊
ACS CATALYSIS
卷 12, 期 2, 页码 1338-1356出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05495
关键词
lignin; Ni2P catalyst; NiAl-hydrotalcite; hydrodeoxygenation; naphthenes; DFT calculations
资金
- National Key R&D Program of China [2018YFB1501500]
- National Natural Science Foundation of China [21975181, 22178258]
- Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development [E139kf0701]
- State Key Laboratory of Pulp and Paper Engineering (South China University of Technology) [202113]
A strategy for low-temperature synthesis of nickel phosphide catalysts with flower-like porous structures is proposed. These catalysts exhibit high activity and selectivity in the hydrodeoxygenation reaction, converting lignin-derived compounds into alkanes.
A strategy for low-temperature synthesis of hydrotalcite-based nickel phosphide catalysts (Ni2P-Al2O3) with flower-like porous structures was proposed. The in situ reduction of red phosphorus at 500 degrees C enables Ni2P catalysts with small particle size and abundant active and acidic sites, which facilitate the activation of substrates and H-2. In the hydrodeoxygenation of guaiacol, a 100% conversion and 94.5% yield of cyclohexane were obtained over the Ni2P-Al2O3 catalyst under 5 MPa H-2 at 250 degrees C for 3 h. Other lignin-derived phenolic compounds could also afford the corresponding alkanes with yields higher than 85%. Moreover, Ni2P-Al2O3 exhibited high hydrodeoxygenation activity in the deconstruction of more complex wood structures, including lignin oil and real lignin. Among the two different types of Ni sites of Ni(1) and Ni(2) in Ni2P, density functional theory (DFT) calculations showed that the Ni(2) site, highly exposed on the Ni2P-Al2O3 surface, possesses a stronger ability to break C-OH bonds during the hydrodeoxygenation of guaiacol in comparison with the Ni(1) site.
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