海绵铁三金属降解对硝基苯酚的影响因素及催化机理

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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.

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	李方芳
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	雷国元

关键词 ：海绵铁, Pd-(Cu-s-Fe⁰)三金属, 对硝基苯酚(PNP), 降解机理

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).

Key words： sponge iron Pd-(Cu-s-Fe⁰) trimetal p-nitrophenol (PNP) degradation mechanism

收稿日期: 2021-02-04

PACS:

X703.5

基金资助: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）

通讯作者: 雷国元,教授,leiguoyuanhit@126.com E-mail: leiguoyuanhit@126.com

作者简介: 李方芳(1997-),女,湖北荆州人,武汉科技大学硕士研究生,主要从事海绵铁材料降解机理研究.发表论文1篇.

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. 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. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(10): 4670-4676.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I10/4670

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