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纳米Fe/Co合金类Fenton降解盐酸四环素及影响因素
引用本文:李君超,蒋进元,张伟,白璐,李云,许春莲.纳米Fe/Co合金类Fenton降解盐酸四环素及影响因素[J].环境科学研究,2018,31(4):757-764.
作者姓名:李君超  蒋进元  张伟  白璐  李云  许春莲
作者单位:中国环境科学研究院工程设计中心, 北京 100012
基金项目:国家水体污染控制与治理重大科技专项(No.2014ZX07504003);中央级公益性科研院所基本科研业务费专项(No.2015YSKY008)
摘    要:为研究纳米Fe/Co合金对含TCs(盐酸四环素)废水的类Fenton催化性能,以及催化降解体系pH、H2O2投加量和活性成分浸出等因素对催化性能的影响.采用液相还原法制备纳米Fe/Co合金,并通过对比试验探究其类Fenton催化性能,Fe、Co的浸出量及其表面积结构变化与活性之间的关系.添加纳米Fe/Co合金的条件下,采用单因素分析方法研究体系pH、H2O2投加量和初始TCs浓度分别对TCs去除率的影响.结果表明:①在纳米Fe/Co合金制备过程中,添加PVP(聚乙烯吡咯烷酮)不仅能有效防止纳米Fe/Co合金发生团聚,且促进纳米Fe/Co合金比表面积增大(BET为113.8 m2/g).②纳米Fe/Co合金具有拓宽催化体系pH使用范围的优势;在pH为3.0~9.0范围内,纳米Fe/Co合金对30 mg/L TCs的去除率(87.2%~91.7%)远大于FeCl2(0~30.7%)和纳米Fe的去除率(0~28.2%);H2O2投加量超过150 mmol/L后,TCs的去除率达到最佳(86.2%).③纳米Fe/Co合金催化体系中(pH为3.0~11.0),活性成分Fe、Co浸出量分别为0.20~0.35和0.20~1.00 mg/L,均满足我国GB 3838—2002《地表水环境质量标准》,长期使用也不会造成浸出成分(Fe、Co)在环境中大量累积,对生态环境等可能造成的潜在风险大大降低.④纳米Fe/Co合金具有再利用性,催化利用4次后,对TCs的去除效果仍达50.0%以上.研究显示,纳米Fe/Co合金对去除TCs具有较高催化性能和再利用性,利于拓宽催化体系pH使用范围,具有稳定活性成分Fe、Co浓度的优势. 

关 键 词:类Fenton    纳米Fe/Co合金    盐酸四环素
收稿时间:2017/10/25 0:00:00
修稿时间:2018/1/15 0:00:00

Oxidative Degradation of Tetracycline Hydrochloride Using Nano Fe/Co Alloy and H2O2 under Fenton Conditions
LI Junchao,JIANG Jinyuan,ZHANG Wei,BAI Lu,LI Yun and XU Chunlian.Oxidative Degradation of Tetracycline Hydrochloride Using Nano Fe/Co Alloy and H2O2 under Fenton Conditions[J].Research of Environmental Sciences,2018,31(4):757-764.
Authors:LI Junchao  JIANG Jinyuan  ZHANG Wei  BAI Lu  LI Yun and XU Chunlian
Affiliation:Research Center of Environmental Engineering Design, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
Abstract:In order to investigate the Fenton-like catalytic activity of nano Fe/Co alloy to wastewater which contained tetracycline hydrochloride (TCs), and the effects of pH, H2O2, active ion leaching and other factors on the catalytic activity, the nano Fe/Co alloy was prepared using liquid reduction method. In addition,we explored the Fenton-like catalytic properties, the leaching amount of Fe and Co, and the relationship between changes in structural surface area and catalytic activity. Under the conditions of adding nano Fe/Co alloy, the influences of system pH value, H2O2 additions and initial TCs concentration on the catalytic degradation efficiency of TCs were studied using single factor analysis. The results showed that:(1) In the preparation of nano Fe/Co alloy, the additions of polyvinyl pyrrolidone (PVP) could effectively prevent the agglomeration of nano Fe/Co alloy and promote the increase of specific surface area of nano Fe/Co alloy (BET=113.8 m2/g). (2) Nano Fe/Co alloy had the advantage in widening pH use range in the catalytic system. At pH=3.0-9.0 range, the removal efficiency of nano Fe/Co alloy (87.2%-91.7%) to 30 mg/L TCs solution was greater than those of FeCl2 (0-30.7%) and nano Fe (0-28.2%). The removal rate of TCs (86.2%) was the best as the addition of H2O2 exceeded 150 mmol/L. (3) For the nano Fe/Co alloy catalytic system (pH=3.0-11.0), the leaching concentrations of Fe and Co were 0.20-0.35 mg/L and 0.20-1.00 mg/L respectively, meeting the requirements of GB 3838-2002 ''Environmental Quality Standards for Surface Water'', long-term use will not result in a large accumulation of leaching components (Fe, Co) in the environment, potentially reducing the potential risks to the ecological environment; (4) Nano Fe/Co alloy had reusability, and the degradation of TCs was still above 50.0% after 4 times of catalytic utilization. In conclusion, the nano Fe/Co alloy had higher catalytic performance and reusability for degradation of TCs, and the advantages in broadening the use of catalytic system pH range, with the stability of the active ingredient Fe, Co concentration advantage.
Keywords:like-Fenton  nano Fe/Co alloy  tetracycline hydrochloride
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