氢等离子体制备Pd/GO-P催化材料及其催化还原对硝基苯酚性能  

Hydrogen Plasma Synthesis of Pd/GO-P and Its Performance for Catalytic Reduction of p-Nitrophenol

作　　者：赵玲玉 赵可鑫 张秀玲[2] 滑跃 底兰波[2] ZHAO Lingyu;ZHAO Kexin;ZHANG Xiuling;HUA Yue;DI Lanbo(College of Environmental and Chemical Engineering,Dalian University,Dalian 116622,China;College of Physical Science and Technology,Dalian University,Dalian 116622,China)

机构地区：[1]大连大学环境与化学工程学院,辽宁大连116622 [2]大连大学物理科学与技术学院,辽宁大连116622

出　　处：《石油学报（石油加工）》2023年第5期1059-1069,共11页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(52077024,21773020,21673026);兴辽英才计划项目(2022RJ16);工业装备结构分析国家重点实验室课题(GZ21105);云南警官学院云南省刑事科学技术重点实验室课题(YJKF003);辽宁省教育厅青年基金项目(LJKQZ20222434)资助。

摘　　要：通过简单过量浸渍法制备氧化石墨(GO)载钯前驱体(Pd/GO-As),采用氢等离子体处理制备氧化石墨载钯催化材料(Pd/GO-P),并以对硝基苯酚(4-NP)还原为模型反应,考察放电电压和放电时间对制备Pd/GO-P催化材料构效关系的影响。研究结果表明:当放电电压为17 kV、放电时间为6 min时,制备的Pd/GO-P催化材料表现出最佳的催化还原4-NP活性,反应速率常数高达1.93 min^(-1),相应的浓度归一化速率常数为1038 L/(min·g),是氢气热还原制备样品活性的9.6倍。这是由于该条件下制备的Pd/GO-P催化材料具有缺陷密度高、含氧官能团丰富、金属活性组分粒径小、分散性好、金属-载体相互作用强等特点,有利于4-NP的吸附和催化活性的提高。氢等离子体是一种快速、绿色、高效、环保的调控制备Pd/GO-P催化材料的方法,对脱除废水中4-NP具有重要参考作用。A graphite oxide-supported palladium precursor(Pd/GO-As)was prepared simply by excess impregnation method,and graphite oxide(GO)-supported Pd catalysts(Pd/GO-P)were treated and prepared using hydrogen plasma;meanwhile,the effects of discharge voltage and discharge time on the structure-activity relationship of Pd/GO-P catalysts were investigated based on the reaction model of p-nitrophenol(4-NP)reduction.The results indicate that when the following preparation conditions are met:the discharge voltage of 17 kV and discharge time of 6 min,Pd/GO-P catalysts display the best catalytic activity for 4-NP reduction,which is about 9.6 times the activity of those prepared by conventional thermal reduction method;specifically,the reaction rate constant is as high as 1.93 min^(-1),and the corresponding concentration-normalized rate constant is 1038 L/(min·g).This can be ascribed to that the prepared Pd/GO-P catalysts prepared under such conditions have the characteristics of high defect-density,abundant oxygen-containing groups,small-sized and highly dispersed metal active components,and strong metal-support interaction,which is conducive to 4-NP adsorption and the improvement of catalytic activity.This work has proved that hydrogen plasma is a rapid,green,highly-efficient and environment-friendly method for regulatory preparation of Pd/GO-P catalysts,which is of significant reference for removing 4-NP in wastewater.

关 键 词：氧化石墨载钯 氢等离子体 对硝基苯酚还原 介质阻挡放电 催化活性 

分 类 号：O643[理学—物理化学]