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化学学报
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化学学报 ›› 2009, Vol. 67 ›› Issue (23): 2650-2654. 上一篇    下一篇

研究论文

Keggin型杂多阴离子PW11O39Fe(III)(H2O)4-电催化降解硝基苯

华英杰a，王崇太*,a,b，童叶翔c，张大帅a，张 奇a ，谷铁安a，胡 佩a   

  1. (a海南师范大学化学与化工学院 海口 571158) (b海南省热带药用植物化学重点实验室 海口 571158) (c中山大学化学与化工学院 广州 510275)
  • 投稿日期:2009-05-13 修回日期:2009-08-10 发布日期:2009-10-09
  • 通讯作者: 王崇太 E-mail:wct581@sina.com

Electrocatalytic Degradation of Nitrobenzene with Keggin-type Fe(Ⅲ)-Substituted Heteropolyanion PW11O39Fe(III)(H2O)4−

Hua, Yingjiea，Wang, Chongtai*,a,b，Tong, Yexiangc，Zhang, Dashuaia ，Zhang, Qia，Gu, Tieana，Hu, Peia   

  1. (a School of Chemistry and Chemical Engineering, Hainan Normal University, Haikou 571158) (b Key Laboratory of Tropical Medicinal Plant Chemistry of Hainan Province, Haikou 571158) (c School of Chemistry and Chemical Engineering, Sun Yat-sen University, Guangzhou 510275)
  • Received:2009-05-13 Revised:2009-08-10 Published:2009-10-09
  • Contact: chongtai wang E-mail:wct581@sina.com

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以Keggin型铁取代杂多阴离子PW11O39Fe(III)(H2O)4－ (PW11Fe)代替传统电芬顿(electro-Fenton)方法中的Fe3＋作为电催化剂, 构成一个新颖的电催化体系并用于中性水溶液中硝基苯的降解. 结果表明, 含有1.0 mmol•L－1硝基苯和1.0 mmol•L－1 PW11Fe的混合磷酸盐溶液(pH 6.86), 在－0.5 V电位和60 mL•min－1 O2流速下反应100 min, 硝基苯便完全降解. 降解的准一级表观速率常数与硝基苯的初始浓度有关, 当硝基苯的初始浓度为1.0, 2.0和5.0 mmol•L－1时, kobs分别为7.18×10－2, 3.57×10－2和1.47×10－2 min－1. 降解反应100 min的TOC(有机碳总量)去除率约为35%, 表明硝基苯的降解过程伴随着矿化.

关键词: 铁取代杂多阴离子, 电催化, 硝基苯降解, 矿化率

A novel system constituted by Keggin-type iron-substituted heteropolytungstate anion PW11O39Fe(III)(H2O)4－ [PW11Fe] was applied to degrade nitrobenzene (NB) in a neutral aqueous solution. Experimental results showed that a complete NB degradation was obtained in less than 100 min in a pH 6.86 mixed phosphate solution containing 1.0 mmol•L－1 NB and 1.0 mmol•L－1 PW11Fe at the potential of －0.5 V and 60 mL•min－1 O2 flow rate. The observed quasi-first order rate constant kobs of NB degradation related with NB initial concentration, which was determined to be 7.18×10－2, 3.57×10－2 and 1.47×10－2 min－1 at the initial concentration of 1.0, 2.0 and 5.0 mmol•L－1, respectively. Ca. 35% TOC (total organic carbon) removal obtained at 100 min reaction time indicated that the process of NB degradation was accompanied by partial mineralization.

Key words: Fe(III)-substituted heteropolyanion, electrocatalysis, nitrobenzene degradation, mineralization