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海绵铁三金属降解对硝基苯酚的影响因素及催化机理
引用本文:李方芳,鞠勇明,邓东阳,贾文超,丁紫荣,雷国元.海绵铁三金属降解对硝基苯酚的影响因素及催化机理[J].中国环境科学,2021,41(10):4670-4676.
作者姓名:李方芳  鞠勇明  邓东阳  贾文超  丁紫荣  雷国元
作者单位:1. 武汉科技大学资源与环境工程学院, 湖北 武汉 430000;2. 生态环境部华南环境科学研究所, 广东 广州 510655;3. 生态环境部南京环境科学研究所, 江苏 南京 210042
基金项目:国家重点研发计划(2019YFE0111100);广东省国际合作项目(2018A050506045);广东省基础与应用基础研究基金资助项目(2020A1515010969);公益性科研院所专项项目(GYZX210301)
摘    要:通过超声置换反应制备钯铜共修饰海绵铁三金属催化剂(Pd-(Cu-s-Fe0)),研究了三金属负载顺序、金属负载量、材料投加量以及重复利用对材料降解对硝基苯酚(PNP)的影响,并利用扫描电子显微镜(SEM)和X射线光电子能谱(XPS)表征材料表面结构特征.结果表明,Pd-(Cu-s-Fe0)催化活性高于Cu-(Pd-s-Fe0)和(Cu-Pd)-s-Fe0;Cu和Pd的最佳负载量分别为5%和0.025%.在100mL初始浓度为100mg/L的PNP溶液中投加3g Pd-(Cu-s-Fe0)并超声反应30min,PNP的降解率超过80%,降解反应基本符合一级动力学方程;Pd-(Cu-s-Fe0)材料循环利用4次表现出良好的循环利用性能.此外,PNP的主要催化还原产物是对氨基苯酚(PAP),主要的反应路径是催化还原反应.

关 键 词:海绵铁  Pd-(Cu-s-Fe0)三金属  对硝基苯酚(PNP)  降解机理  
收稿时间:2021-02-04

Study on influencing factors and catalytic mechanism of p-nitrophenol degradation with sponge iron-based tri-metals
LI Fang-fang,JU Yong-ming,DENG Dong-yang,JIA Wen-chao,DING Zi-rong,LEI Guo-yuan.Study on influencing factors and catalytic mechanism of p-nitrophenol degradation with sponge iron-based tri-metals[J].China Environmental Science,2021,41(10):4670-4676.
Authors:LI Fang-fang  JU Yong-ming  DENG Dong-yang  JIA Wen-chao  DING Zi-rong  LEI Guo-yuan
Institution:1. Department of Resources and Environmental Engineering, Wuhan University of Science and Technology, Wuhan 430000, China;2. South China Institute of Environmental Science, Ministry of Ecology and Environment of the People's Republic of China, Guangzhou 510655, China;3. Nanjing Institute of Environmental Science, Ministry of Ecology and Environment of the People's Republic of China, Nanjing 210042, China
Abstract:Pd-(Cu-s-Fe0) trimetals were synthesized adopting with displacement reactions under ultrasonic conditions, and the surface structure of the aforementioned materials was further characterized with scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). Moreover, the effects of noble metal loading sequence, the loading amount, input dosage and recycling reuse for the degradation of p-nitrophenol (PNP) was studied in detail. The experimental results show that the catalytic activity of Pd-(Cu-s-Fe0) was higher than that of Cu-(Pd-s-Fe0) and (Cu-Pd)-s-Fe0. The loading amounts of Cu and Pd were optimized as 5% and 0.025%, respectively. Under the optimized conditions including 30g/L of Pd-(Cu-s-Fe0), the removal content of PNP (100mL, initial concentration of 100mg/L) reached more than 80% after 30min of ultrasonic reactions, and the degradation reactions conformed to a pseudo-first-order kinetics equation. Furthermore, after 4times of recycling tests, Pd-(Cu-s-Fe0) showed good recycling performance. Based on the UV-visible spectral variations and high-performance liquid chromatography, we proposed the degradation mechanism mainly via catalytic reductions of PNP into p-aminophenol (PAP).
Keywords:sponge iron  Pd-(Cu-s-Fe0) trimetal  p-nitrophenol (PNP)  degradation mechanism  
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