竹浆纤维素转化制低碳多元醇反应中有机氮对金属催化剂稳定性影响的研究

采用等体积浸渍法制备了一系列多孔竹炭负载的有机氮掺杂的镍钨催化剂，并将其应用于催化竹浆纤维氢解制C_2，3多元醇反应。有机氮源与催化剂前驱体中Ni²⁺络合，高温煅烧时载体表面碳、氮和金属离子相互作用后生成一定量的C₃N₄、氮化物和合金物相。通过XRD、XPS和TEM等表征手段分析了催化剂Ni-W/MBC表面物理化学性质与催化活性间的关系。结果表明，除了金属镍、氧化钨物相外，表面还含有Ni-W合金（NiWO₄为主）；金属粒子表面包围了一层石墨化C₃N₄物相。XPS分析表明，有机氮源高温分解反应后形成了C₃N₄物相。在反应条件下，15% Ni-20% W/MBC@M-0.25催化剂得到乙二醇收率为55.8%，而未添加有机氮源的催化剂15% Ni-20% W/MBC获得的乙二醇收率仅为36.9%。催化剂稳定性实验结果表明，Ni-W合金和C₃N₄物相的形成显著增强了Ni-W/MB催化剂的稳定性，延长了催化剂寿命。

Organic nitrogen promotes stability of metallic catalysts in conversion of bamboo pulp to low carbon polyols

Herein, the synthesis and performance of a novel and stable catalyst capable of facile hydrolysis of bamboo pulp were reported. Based on adopting complex agent to have a complex reaction with Ni²⁺ cations, the graphitic g-C₃N₄ phase and nitride phases were formed eventually. The interaction among metals and C, N atoms was analyzed by XRD and XPS. Some Ni-W alloys (mainly NiWO₄ was included) were formed besides metallic Ni⁰ and tungsten species characterized. Particles on the surface of 15%Ni-20%W/MBC@M-0.25 catalyst exhibited homogeneous distribution and surrounded by disordered C₃N₄ layer characterized by TEM. Besides, the organic N sources were decomposed and the C₃N₄ phase with high hydrothermal property was formed simultaneously. For catalytic efficiency, 15%Ni-20%W/MBC@M-0.25 catalyst acquired the highest EG yield of 55.8% compared to 36.9% via 15%Ni-20%W/MBC catalysts. The carbon supports and organic nitrogen sources demonstrated great influence on catalytic efficiency. Catalyst recycle experiments implied that Ni-W/MBC@M-0.25 could remain relative stable under this catalytic reaction condition. The Ni-W alloys and the C₃N₄ phase were deduced as the main contributors to maintain the catalyst stability.