活性碳纤维耦合喹啉铁的pH-tolerant性能研究
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摘要
pH值适应范围窄一直是制约芬顿反应发展的技术瓶颈,因此,开发pH-tolerant类芬顿催化剂成为环境催化领域的研究热点和难点。采用活性碳纤维(ACFs)耦合喹啉铁(QuFe)制得一种新型pH-tolerant类芬顿催化纤维(QuFe@ACFs),该催化纤维在中性条件下可以活化双氧水有效降解活性艳红M-3BE。采用自由基捕获剂邻苯二胺,结合电子顺磁共振波谱、紫外-可见光谱等对催化纤维的重复稳定性进行了重点考察。结果显示,QuFe@ACFs在pH值为3~9范围内均具有良好的催化性能和重复使用性,表现出了优异的pH-tolerant性能。QuFe@ACFs制备方法简单,巧妙解决了制约传统芬顿反应发展的技术瓶颈,为制备新一代高活性pH-tolerant芬顿催化剂提供了新思路。
The application of Fenton reaction is restricted to a narrow pH range(2-3.5),which has long been a technological bottleneck.Therefore,the development of a pH-tolerant Fenton-like catalyst is an active and challenging research front in the field of environmental catalysis.In this work,the pH-tolerant performance of the novel Fenton-like catalytic fibers(QuFe@ACFs)based on activated carbon fibers(ACFs)coupled with 8-hydroxyquinoline ferric(QuFe)was evaluated by a simple impregnation method.The UV-Vis spectroscopy measurements showed that the reactive brilliant red M-3BE(RR M-3BE)was completely degraded in 32 min.Probe compound O-phenylenediamine combined with electron paramagnetic resonance(EPR)spectroscopy and UV-Vis spectroscopy were employed to demonstrate the catalytic stability of QuFe@ACFs,and the experimental results showed that QuFe@ACFs exhibited excellent catalytic ability and recycle utilization performance across a wide pH range from 3to 9,brought remarkable pH-tolerant performance.To sum up,the QuFe@ACFs prepared by an extremely simple impregnation method,breaks the technological bottleneck for Fenton treatment,providing new ideas for preparing novel pH-tolerant Fenton-like catalysts with excellent catalytic activity.
The application of Fenton reaction is restricted to a narrow pH range(2-3.5),which has long been a technological bottleneck.Therefore,the development of a pH-tolerant Fenton-like catalyst is an active and challenging research front in the field of environmental catalysis.In this work,the pH-tolerant performance of the novel Fenton-like catalytic fibers(QuFe@ACFs)based on activated carbon fibers(ACFs)coupled with 8-hydroxyquinoline ferric(QuFe)was evaluated by a simple impregnation method.The UV-Vis spectroscopy measurements showed that the reactive brilliant red M-3BE(RR M-3BE)was completely degraded in 32 min.Probe compound O-phenylenediamine combined with electron paramagnetic resonance(EPR)spectroscopy and UV-Vis spectroscopy were employed to demonstrate the catalytic stability of QuFe@ACFs,and the experimental results showed that QuFe@ACFs exhibited excellent catalytic ability and recycle utilization performance across a wide pH range from 3to 9,brought remarkable pH-tolerant performance.To sum up,the QuFe@ACFs prepared by an extremely simple impregnation method,breaks the technological bottleneck for Fenton treatment,providing new ideas for preparing novel pH-tolerant Fenton-like catalysts with excellent catalytic activity.
引文
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[17]Fang Yanfen,Deng Anping,Huang Yingping.Determination of hydroxyl radical in Fenton system[J].Chinese Chemical Letters,2009,20:1235-1240.
[18]Yao Yuyuan,Wang Lie,Sun Lijie,et al.Efficient removal of dyes using heterogeneous Fenton catalysts based on activatedcarbon fibers with enhanced activity[J].Chemical Engineering Science,2013,101:424-431.
[2]Liu Zhenzhong,Deng Huiping,Tao Meijun.Decomposition kinetics of trichlorophenol by modified activated carbon combined with hydrogen peroxide[J].Journal of Functional Materials,2014,5:05139-05143.
[3]Silva M R A,Trov′o A G,Nogueira R F P.Degradation of the herbicide tebuthiuron using solar photo-Fenton process and ferric citrate complex at circumneutral pH[J].Journal of Photochemistry and Photobiology A:Chemistry,2007,191:187-192.
[4]Huang Wenyu,Brigante Marcello,Wu Feng,et al.Assessment of the Fe(Ⅲ)-EDDS complex in Fenton-like processes:from the radical formation to the degradation of bisphenol A[J].Environmental Science Technology,2013,47:1952-1959.
[5]Nam S,Renganathan V G P.Substituent effects on azo dye oxidation by the FeⅢ-EDTA-H2O2 system[J].Chemosphere,2001,45:59-65.
[6]Ramirez J H,Costa C A,Madeira L M,et al.Fenton-like oxidation of orangeⅡsolutions using heterogeneous catalysts based on saponite clay[J].Applied Catalysis B:Environmental,2007,71:44-56.
[7]Rodriguez A,Ovejero G,Sotelo J L,et al.Heterogeneous Fenton catalyst supports screening for mono azo dye degradation in contaminated wastewaters[J].Industrial&Engineering Chemistry Research,2010,49:498-505.
[8]Cheng Mingming,Ma Wanhong,Li Jing,et al.Visiblelight-assisted degradation of dye pollutants over Fe(Ⅲ)-loaded resin in the presence of H2O2at neutral pH values[J].Environmental Science Technology,2004,38:1569-1575.
[9]Duarte F,Maldonado-hodar F J,Madeira L M.Influence of the particle size of activated carbons on their performance as Fe supports for developing Fenton-like catalysts[J].Industrial Engineering Chemistry Research,2012,51:9218-9226.
[10]Chen Wenxing,Lu Wangyang,Yao Yuyuan,et al.Highly efficient ecomposition of organic dyes by aqueous-fiber phase transfer and in situ catalytic oxidation using fiber-supported cobalt phthalocyanine[J].Environmental Science Technology,2007,41:6240-6245.
[11]Huang Zhenfu,Bao Haiwei,Yao Yuyuan,et al.Novel green activation processes and mechanism of peroxymonosulfate based on supported cobalt phthalocyanine catalyst[J].Applied Catalysis B:Environmental,2014,154-155:36-43.
[12]Lu Wangyang,Chen Wenxing,Li Nan,et al.Oxidative removal of 4-nitrophenol using activated carbon fiber and hydrogen peroxide to enhance reactivity of metallophthalocyanine[J].Applied Catalysis B:Environmental,2009,87:146-151.
[13]Wang Lie,Yao Yuyuan,Sun Lijie,et al.Activation of hydrogen peroxide by activated carbon fibers coupled with Fe(Ⅲ)-citrate for degradation of dyes at neutral pH[J].Acta Chimica Sinica,2013,71:1633-1638.
[14]Wang Lie,Yao Yuyuan,Zhang Zhanhao,et al.Activated carbon fibers as an excellent partner of Fenton catalyst for dyes decolorization by combination of adsorption and oxidation[J].Chemical Engineering Journal,2014,251(1):348-354.
[15]Yao Yuyuan,Mao Yajun,Huang Qunfeng,et al.Enhanced decomposition of dyes by hemin-ACF with significant improvement in pH tolerance and stability[J].Journal of Hazardous Materials,2014,264:323-331.
[16]Sun Lijie,Yao Yuyuan,Wang Lie,et al.Efficient removal of dyes using activated carbon fibers coupled with 8-hydroxyquinoline ferric as a reusable Fenton-like catalyst[J].Chemical Engineering Journal,2014,240:413-419.
[17]Fang Yanfen,Deng Anping,Huang Yingping.Determination of hydroxyl radical in Fenton system[J].Chinese Chemical Letters,2009,20:1235-1240.
[18]Yao Yuyuan,Wang Lie,Sun Lijie,et al.Efficient removal of dyes using heterogeneous Fenton catalysts based on activatedcarbon fibers with enhanced activity[J].Chemical Engineering Science,2013,101:424-431.