Ce^(3+)与Cu^(2+)协同强化芬顿体系氧化苯酚的效能与机制研究  

Synergistic Enhancement on Oxidation of Phenol by Fenton Processes by Adding Ce^(3+) and Cu^(2+) Ions

作　　者：张剑桥[1] 迟惠中 宋阳[1] 罗从伟[1] 江进[1] 马军[1] 

机构地区：[1]哈尔滨工业大学市政环境工程学院,哈尔滨150090

出　　处：《环境科学》2016年第8期3067-3072,共6页Environmental Science

基　　金：国家科技支撑计划项目(2012BAC05B02)

摘　　要：研究了Ce^(3+)与Cu^(2+)协同强化芬顿体系在不同初始条件下对水中苯酚的氧化效能与机制.结果表明,在p H适用范围的宽度和H_2O_2浓度变化方面,Ce^(3+)/Cu^(2+)/Fe^(2+)/H_2O_2体系比传统的芬顿体系更具有优势,该体系在p H=5.0、H_2O_2浓度为2.0mmol·L-1的条件下,仍可以对苯酚保持相对较高的氧化效能;Cu^(2+)可能会借助反应过程中的中间产物(醌类物质)生成Cu+,Cu+催化H_2O_2分解生成·OH,Ce^(3+)可能促进体系内醌类物质的形成,加快Fe^(3+)与Fe^(2+)的循环效能,在一定程度上提高了芬顿体系中H_2O_2分解生成·OH的速率,说明Cu^(2+)与Ce^(3+)对芬顿体系的强化作用具有协同性;自由基终止剂依然可以抑制Ce^(3+)、Cu^(2+)强化的芬顿体系对苯酚的降解,由此说明体系中起到氧化作用的活性物种仍然是羟基自由基(·OH).Synergistic effect of Ce3＋and Cu2＋on the oxidation efficiency of phenol in different initial p H and H2O2 concentrations by Fenton processes was studied. The experiment results illustrated that Ce3＋/ Cu2＋/ Fe2＋/ H2O2 system had a wider scope of application than Fenton process in the aspect of p H and H_2O_2 concentration. Phenol was still efficiently degraded by Ce3＋/ Cu2＋/ Fe2＋/ H2O2 at a higher p H（ p H = 5. 0） and a higher H_2O_2concentration（ 2. 0 mmol·L-1）. In addition,Cu2＋could react with quinone-like substrates,the oxidation intermediates of phenol,to produce Cu＋,which could catalyze the decomposition of H2O2 to form·OH,while Ce3＋could accelerate the formation of quinone-like substrates and facilitate the cycling of Fe3＋and Fe2＋,to enhance the decomposition of H2O2 to form·OH,the mechanism analysis illuminated the synergy of Ce3＋and Cu2＋. The reactive species in Ce3＋/ Cu2＋/ Fe2＋/H2O2 system was still proved to be·OH,resulting from the scavenging experiments by adding different radical scavengers.

关 键 词：三金属芬顿体系 铈离子 苯酚 羟基自由基 协同强化 醌类物质 

分 类 号：X703.1[环境科学与工程—环境工程]