As a renewable carbon resource, biomass is of great significance for converting it into high value-added chemicals such as polyols, aromatic hydrocarbons and alkanes. Nickel-based catalysts have been shown to have high catalytic activity in reactions such as hydrogenation, hydrocracking, and hydrodeoxygenation of biomass. However, in the reaction medium for biomass conversion (strong acid, high temperature, hydrothermal), most nickel-based catalysts cannot be stably present, which is mainly due to the fact that low-level nickel-based catalytically active species are prone to dissolution in acid solutions. The process of loss and aggregation grows up, which leads to the loss of activity of the catalyst. This drawback has also become a huge obstacle to limiting the application of nickel-based catalysts in biomass conversion reactions. Therefore, there is an urgent need to develop a new acid-resistant, stable nickel-based catalyst for use in the field of biomass hydrogenation.
Recently, the team of academicians Wang Aiqin and Zhang Tao of the Center for Aerospace Catalysis and New Materials of the Dalian Institute of Chemicals, Chinese Academy of Sciences, for the first time carried out research on monoatomic catalysts and biomass conversion, and for the first time carried high-metal loadings of nickel-nitrogen-carbon (Ni-NC). Monoatomic catalysts have been used in biomass conversion reactions and have made significant progress. The related work was published in the form of communication on Angew. Chem. Int. Ed. and was selected as a hot paper.
The research team prepared a Ni-NC monoatomic catalyst with a nickel loading of up to 7.5 wt% and applied it to cellulose conversion to produce polyols. Compared to activated carbon-supported nickel nanoparticle catalysts (Ni/AC), Ni-NC monoatomic catalysts exhibit excellent durability under severe conditions of high temperature, high pressure, strong acid, and high temperature water and heat, and the catalyst can be recycled more than 7 times. No significant reduction in activity and mononuclear aggregation were observed. Through in-depth characterization, the researchers successfully resolved that the Ni-NC monoatomic catalyst's active center is a nickel mono atom and four pyridinic nitrogens coordinate to form a distorted quasi-plane Ni-N4 group, and the fifth pyridinium nitrogen is The direction of the vertical axis is weakly adsorbed on the nickel center to form a Ni-N5 structure, and hydrogen molecules can be effectively activated on the active center. This progress has important implications for the conversion of biomass into high value-added chemicals such as cosmetics (polyols), polyester fibers (diols/diacids/PX), and aviation kerosene (aromatics).
The above research work has been funded by the National Natural Science Foundation of China, the Ministry of Science and Technology, the Special Initiative for Strategic Pilot of the Chinese Academy of Sciences and the Collaborative Innovation Center for Energy Materials Chemistry of the Ministry of Education.
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