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Pd/C-N@SiO2催化剂的制备、表征及其催化松香歧化反应性能

Preparation, Characterization and Catalytic Performance of Pd/C-N@SiO2 Catalyst for Disproportionation Reaction of Rosin

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【作者】 黄振中解从霞于凤丽袁冰

【Author】 HUANG Zhenzhong;XIE Congxia;YU Fengli;YUAN Bing;College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology;

【通讯作者】 解从霞;

【机构】 青岛科技大学化学与分子工程学院

【摘要】 通过典型的溶胶-凝胶聚合方法合成了具有空心结构的N掺杂两亲性中空纳米材料C-N@SiO2,并选择Pd为活性组分,通过浸渍法负载在两亲性中空纳米材料上得到Pd/C-N@SiO2催化剂,并用于催化松香歧化反应。采用SEM、TEM、N2脱附-吸附、XPS、XRD等手段对催化剂进行了一系列的分析与表征,结果表明:C-N@SiO2催化剂具有较大的比表面积(226 m2/g)和孔径(3.85 nm),具有明显的中空结构,有利于松香分子的进入和歧化反应的进行。掺杂的N有利于金属Pd的锚定,分析表明Pd被成功负载到了C-N@SiO2材料上,材料的两亲性提高了催化剂的稳定性和分散性。催化剂Pd/C-N@SiO2对松香歧化反应表现出良好的催化活性,其催化活性超过市售的Pd/C催化剂。1 g松香原料,在250℃、氮气气氛、水/油体积比为3∶12(总量15 mL)、反应时间3.5 h、催化剂用量20 mg的条件下,脱氢枞酸的GC含量达到53.3%,枞酸的GC含量为0.7%。Pd/C-N@SiO2催化剂具有良好的稳定性和重复使用性能,重复使用5次时脱氢枞酸的GC含量仍达到47.1%,催化活性没有明显下降。

【Abstract】 N-doped amphiphilic hollow nanomaterials C-N@SiO2 with hollow structure was synthesized by a typical sol-gel polymerization method. Pd was selected as the active component and supported on amphiphilic hollow nanomaterials by impregnation method to obtain Pd/C-N@SiO2 catalyst, which was used to catalyze the disproportionation reaction of rosin. The catalyst was analyzed and characterized by SEM, TEM, N2 adsorption-desorption, XPS, XRD and other characterization methods. The results showed that the C-N@SiO catalyst had large specific surface area(226 m2/g) and pore diameter(3.85 nm) with hollow structure, which were conducive to the entry of rosin molecules and the disproportionation reaction. The doped N was conducive to the anchoring of metal Pd, and the analysis indicated that Pd was successfully loaded on the C-N@SiO2 materials, and the amphiphilicity of the material improved the stability and dispersion of the catalyst. The catalytic activity of Pd/C-N@SiO2 for the disproportionation reaction of rosin, and its catalytic activity exceeded the commercially available Pd/C catalysts. The GC content of dehydroabietic acid reached 53.3% and the content of abietic acid was 0.7% under the conditions of 250 ℃, nitrogen atmosphere, water-oil volume ratio of 3 ∶12(with a total volume of 15 mL), a reaction time of 3.5 h, a catalyst dosage of 20 mg and 1 g rosin raw material. The Pd/C-N@SiO2 catalyst had good stability and reusability. The GC content of dehydroabietic acid still reached 47.1% after 5 times of reuse, and there was no significant decline in the catalytic activity.

【基金】 国家自然科学基金资助项目(32071710);江苏省生物质能源与材料重点实验室开放基金项目(JSBEM201901)
  • 【文献出处】 林产化学与工业 ,Chemistry and Industry of Forest Products , 编辑部邮箱 ,2025年01期
  • 【分类号】TQ645.94;O643.36
  • 【下载频次】104
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