近临界水中杂多酸锌盐催化氧化降解4,4′-二溴联苯

上海大学学报(自然科学版) ›› 2010, Vol. 16 ›› Issue (5): 482-487.

近临界水中杂多酸锌盐催化氧化降解4,4′-二溴联苯

上海大学环境与化学工程学院，上海 200444

收稿日期:2010-04-12 出版日期:2010-10-30 发布日期:2010-10-30
通讯作者: 陈晋阳(1971～)，男，教授，研究方向为超临界流体技术与固体废弃物处理. E-mail:chenjy@shu.edu.cn
基金资助:
上海市教委科研创新基金资助项目（09YZ30）

Subcritical Water Oxidative Degradation of 4,4′-dibromobiphenyl with Heteropoly Zinc Salts

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China

Received:2010-04-12 Online:2010-10-30 Published:2010-10-30

摘要/Abstract

摘要：

使用模板浸渍法制备两种杂多酸锌盐Zn_1.2H_1.8PW₁₂O₄₀和Zn_1.1H_1.9PMo₁₂O₄₀.利用它们作为催化剂，进行了近临界水中4,4′-二溴联苯（4,4′-DBB）氧化降解的实验研究，其中Zn_1.2H_1.8PW₁₂O₄₀具有很好的氧化降解效果，并且稳定性很好.因此，采用Zn _1.2H_1.8PW₁₂O₄₀为催化剂，研究了近临界水中4,4′-DBB氧化降解的工艺条件与动力学.优化工艺条件为物料质量比m(H₂O₂)∶m(4,4′-DBB)=200∶1，反应温度320 ℃，反应压力11.9 MPa，反应时间15 min，在此工艺条件下反应后水样的化学需氧量（chemical oxygen demand,COD）为55.9 mg/L，达到了GB 8978—1996的排放要求.反应动力学的研究结果显示，4,4′-DBB在近临界水中催化氧化降解的反应级数为1.70，表观活化能为44.04 kJ/mol.

关键词: 杂多酸锌盐；4,4′-二溴联苯；近临界水氧化；催化；化学需氧量

Abstract:

Two heteropoly zinc salts of Zn_1.2H_1.8PW₁₂O₄₀and Zn_1.1H_1.9PMo₁₂O₄₀are prepared by template impregnation. They are used as catalyst to oxidative degradation of 4,4′-dibromobiphenyl (4,4′-DBB) in subcritical water. Zn_1.2H_1.8PW₁₂O₄₀pays better role on accelerating degradation rate and shows enough stability. Thus oxidative degradation and the kinetics of 4,4′-DBB in subcritical water are investigated using Zn_1.2H_1.8PW₁₂O₄₀ as catalyst. The optimal experiment conditions are obtained as follows: m(H₂O₂)∶m(4,4′-DBB)= 200∶1, temperature of 320 ℃, pressure of 11.9 MPa, and reaction time of 15 min. Under the optimal condition, chemical oxygen demand （COD） of water sample after reaction can be down to 55.9 mg/L, which meets the Chinese National Standard GB 8978—1996. The order of catalytic oxidation degradation kinetic of 4,4′-DBB in subcritical water is 1.70, and the apparent activation energy is 44.04 kJ/mol. 

Key words: heteropoly zinc salt; 4,4′-dibromobiphenyl; subcritical water oxidation; catalysis; chemical oxygen demand (COD)

中图分类号:

X 703

陈晋阳李志阮如意刘桂洋. 近临界水中杂多酸锌盐催化氧化降解4,4′-二溴联苯[J]. 上海大学学报(自然科学版), 2010, 16(5): 482-487.

CHEN Jin-Yang, LI Zhi, RUAN Ru-Yi, LIU Gui-Yang. Subcritical Water Oxidative Degradation of 4,4′-dibromobiphenyl with Heteropoly Zinc Salts[J]. Journal of Shanghai University（Natural Science Edition）, 2010, 16(5): 482-487.

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