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One-step efficient non-hydrogen conversion of cellulose into γ-valerolactone over AgPW/CoNi@NG composite

Journal 2020 · IF 16.683 · 发表于 2020 年 11 月 20 日
作者: Shanhui Zhu,Huan Liu,Sen Wang,Xiaoqing Gao,Pengfei Wang,Jianguo Wang,Weibin Fan
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摘要

One-step efficient conversion of cellulose into value-added γ-valerolactone (GVL) is of great interest because it not only integrates complex tandem reactions in one-step, but also does not need additional hydrogen sources. To achieve this goal, it is crucial to fabricate high-performance catalyst that can accelerate both hydrolysis of cellulose and further transformation of generated stoichiometric levulinic acid (LA) and formic acid (FA) into GVL. CoNi nanoparticles encapsulated in N-doped thin graphene shell gave GVL yield as high as 55.9 % at 200 °C combined with Ag + -exchanged heteropolyacid (AgPW). This composite catalyst is highly resistant to the corrosion of LA and FA, and hence shows high catalytic stability. LA-adsorption FTIR spectra and DFT calculations indicate that LA and FA can penetrate through shell graphene layers into core CoNi sites via cracks. Compared to H 2 , FA can much more rapidly reduce LA because of its low dissociation energy barrier and high dissociation rate.

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