Pd/rGO催化硝基苯无溶剂加氢合成苯胺
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O643

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国家自然科学基金项目(面上项目,重点项目,重大项目)


Solvent-free reduction of nitrobenzene to aniline catalyzed by Pd/rGO
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    采用氧化石墨烯(GO)、还原石墨烯(rGO)和硝酸活化处理的活性碳(C-HNO3)负载Pd纳米粒子制得了3种Pd基催化剂Pd/GO、Pd/rGO和Pd/C-HNO3。通过XRD、XPS、N2吸附-脱附、SEM、TEM、HRTEM对其进行了表征。以商用Pd/C催化剂(Pd质量分数10%)作为对照,考察3种催化剂催化硝基苯无溶剂加氢的活性和选择性。结果表明,rGO纳米片高效网络结构和Pd纳米粒子之间的良好的耦合作用使得Pd/rGO在3种催化剂中表现出最高的Pd金属比表面积(178.37 m2/g)和分散度(43.75%)。在Pd/rGO催化剂质量浓度为10 g/L,1 MPa H2,90 ℃,5 mL 硝基苯的反应条件下,苯胺的产率随反应时间增加呈上升趋势。反应100 min后,硝基苯完全转化,苯胺产率达到100%。循环使用9次后,Pd/rGO仍可催化硝基苯高效转化获得97.1%的苯胺产率。

    Abstract:

    To further improve catalytic performance under solvent-free conditions, Pd/GO、Pd/rGO and Pd/C-HNO3 were studied with the commercial Pd/C with mass fraction of 10% as the control group. Among them, Pd/rGO exhibited the highest aniline yield within 1 h. Combined with the characterization results of XRD、XPS、N2-adsorption/desorption、SEM、TEM and HRTEM, the coupling effect between Pd nanoparticles and rGO nanosheets is confirmed, which results in the highest Pd specific surface area (178.37 m2/g) and Pd dispersion(43.75%) of Pd/rGO in the three Pd-based catalysts. When Pd/rGO catalyzed the hydrogenation of nitrobenzene in the condition of 10 g/L Pd/rGO,1 MPa H2,90 ℃,5 mL nitrobenzene, the yield of aniline increased with the reaction time. Nitrobenzene was completely transformed and the yield of aniline reached 100% within 100 min. In addition, Pd/rGO exhibited 97.1% aniline yields after recycling tests of nine times.

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周雪珂,周志颖,杨洋,周灿,郑成航,高翔. Pd/rGO催化硝基苯无溶剂加氢合成苯胺[J].精细化工,2022,39(1):0

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  • 收稿日期:2021-07-01
  • 最后修改日期:2021-08-27
  • 录用日期:2021-08-27
  • 在线发布日期: 2021-11-01
  • 出版日期: