研究报告

  • 邓东芝,孙敬雅,郑寿荣.碳包覆Pd/Al2O3催化剂催化4-溴苯酚加氢脱溴的活性和稳定性调控研究[J].环境科学学报,2022,42(12):22-29

  • 碳包覆Pd/Al2O3催化剂催化4-溴苯酚加氢脱溴的活性和稳定性调控研究
  • Activity and stability regulation of carbon-coated Pd/Al2O3 for catalytic hydrodebromination of 4-bromophenol
  • 基金项目:国家重点研发计划(No.2020YFC1807003);国家自然科学基金(No.21577056 )
  • 作者
  • 单位
  • 邓东芝
  • 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
  • 孙敬雅
  • 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
  • 郑寿荣
  • 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
  • 摘要:在污染物液相催化加氢脱卤过程中,提高催化剂的稳定性至关重要.以水热合成法制备了不同碳包覆量的Pd/Al2O3@C催化剂,对催化剂进行了系列表征,并将催化剂应用于4-溴苯酚(4-BP)污染物的催化加氢脱溴反应.表征结果显示碳层提高了Pd/Al2O3的表面疏水性,有利于4-BP在催化剂上的吸附.并且在Pd/Al2O3@C催化剂的碳化过程中,碳还原部分Pd颗粒,并保留部分正价态Pd活性位,增强了4-BP中C-Br键的活化.与Pd/Al2O3相比,碳涂层提高了催化剂的催化活性.但当碳包覆量超过最佳包覆量后,暴露的Pd粒子随碳包覆量的增加而减少,导致活性下降.此外,碳层修饰后,催化剂的稳定性显著提高,从而大大抑制了Pd粒子的团聚和损耗.Pd/Al2O3@C表面的碳涂层对卤素具有较高的耐受性,从而减轻了液相催化加氢脱卤反应中活性中心的中毒.
  • Abstract:Exploring efficient and stable catalysts is of crucial importance for the aqueous catalytic hydrodehalogenation of pollutants. Herein, we prepared the Pd/Al2O3@C catalysts with varied carbon-encapsulation amounts by a hydrothermal approach. The catalysts were characterized and applied for the catalytic hydrodebromination of 4-bromophenol (4-BP). The carbon coating layer improves surface hydrophobicity of Pd/Al2O3@C, favoring 4-BP adsorption on the catalyst. During the carbonization of Pd/Al2O3@C, carbon partially reduces Pd particles with positively charged Pd sites residual, enhancing the activation of C-Br bonds in 4-BP. In comparison with Pd/Al2O3, carbon coating enhances the catalytic activity of Pd/Al2O3; while excessive carbon coating, substantially decrease Pd particle,and thus decreased catalytic activity. Besides, carbon coating remarkedly promoted the stability of Pd/Al2O3 and greatly suppressed the agglomeration and loss of Pd particles. Additionally, Pd/Al2O3@C has exhibited high tolerance towards halogens and thus alleviated the poisoning of active centers during the aqueous catalytic hydrodehalogenation reaction.

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