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Fabrication of immobilized nickel nanoclusters decorated by CxNy species for cellulose conversion to C2,3 oxygenated compounds:Rational design via typical C-and N-sources

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Journal of Energy Chemistry 2020年第11期29卷 25-36页

作者： Zhuqian Xiao Xiaolei Wang Qinqin Yang Chuang Xing Qing Ge Xikun Gai Jianwei Mao Jianbing Ji Zhejiang Provincial Collaborative Innovation Center of Agricultural Biological Resources Biochemical Manufacturing Zhejiang University of Science and TechnologyHangzhou 310023ZhejiangChina School of Chemical Engineering Zhejiang University of TechnologyHangzhou 310023ZhejiangChina

Production of chemicals and fuels from microcrystalline cellulose has inspired scholars’ attention. Deactivation of metallic catalysts including acid leaching and hydrothermal aggregation is still one of the core issues in these systems. To address these problems, we designed and fabricated a series of Ni-W/SiO2 catalysts, which were decorated by CxNy species using C-and N- sources and applied in cellulose conversion to C2,3 oxygenated compounds. The Ni-W/SiO2@CxNy catalysts, underwent complexing and selfassembling process, exhibited special heterojunctions, accompanying strong interactions mainly among Ni phase and CxNy layers. Catalytic results showed that the heterojunctions and outer CxNy layers extensively enhanced productions of hydroxyacetone(HDA) and ethylene glycol(EG) and promoted the hydrothermal stability through prospering in concentration of Lewis pairs from Ni–N—N structure and immobilizing the metallic nanoclusters. 48.25% of EG was yielded under 5.0 MPa H2 pressurized 240 ℃ water for 2.0 h. The Lewis pair further improved the formation of HDA with 20.92% yield. High hydrothermal stability of NiW/SiO2@CxNy catalyst was proved according to the recycling results and trace leaching concentration of Ni and W. This construction of metallic catalysts exploited a new strategy to manufacture extraordinary durability of metallic nanoclusters for cellulose conversion under harsh reaction conditions.

关键词： Cellulose Heterojunction metallic immobilization Leaching-resistance Hydroxyacetone

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