光催化与微生物燃料电池耦合对Cu-EDTA的降解特性

doi:10.11949/0438-1157.20211640

摘要/Abstract

摘要：

工业废水中重金属与有机络合剂形成的重金属络合物是常规水处理方法难以有效去除的污染物之一。光催化氧化是降解水体中重金属络合物的有效方法，但纯TiO₂催化光生电子-空穴对的较高复合效率限制了该技术在降解重金属络合物方面的应用。微生物燃料电池(microbial fuel cell， MFC)可以通过对光催化氧化单元施加电势提升光生电子与空穴分离率的同时有效降低复合效率，最终表现为高效的破络合反应。本文将MFC与光催化氧化进行耦合，在提高Cu-EDTA破络合效率的同时去除Cu²⁺。结果表明单MFC、串联MFC与并联MFC三种耦合方式均能提高光催化单元对Cu-EDTA的去除率，去除率分别为52.6%、73.57%和61.54%；对Cu²⁺的去除效果分别为18.09%、36.87%和21.09%。说明串联MFC耦合方式可以更大程度发挥光催化单元的效率。

关键词: 催化（作用）, 配合物, 光化学, 微生物燃料电池, 自由基, Cu-EDTA

Abstract:

Heavy metal complexes formed by heavy metals and organic complexing agents in industrial wastewater are one of the pollutants that are difficult to effectively remove by conventional water treatment methods. Although photocatalytic oxidation would be a candidate technically for complex degradation, the high recombination ratio of electron-hole pairs generated by TiO₂ limits the application. Microbial fuel cells could suppress recombination of pairs by applying a bias voltage to the photocatalytic unit, which ultimately manifests as an efficient decomplexation reaction. In this work, the coupling of MFC and photocatalytic oxidation was proven to be efficient to improve the removal of Cu-EDTA and Cu²⁺ simultaneously. The results show that the photocatalytic unit matched with single MFC, double MFC connected in series, and double MFC connected in parallel lifted the removal rate of Cu-EDTA up to 52.6%, 73.57%, and 61.54%, respectively, while the removal of Cu²⁺ went to 18.09 %, 36.87% and 21.09%. Accordingly, it was shown that the coupling with MFC connected in series could enhance the removal efficiency of the photocatalytic unit to a greater extent.

Key words: catalysis, complexes, photochemistry, microbial fuel cell, radical, Cu-EDTA

中图分类号:

X 75

张红锐, 张田, 隆曦孜, 李先宁. 光催化与微生物燃料电池耦合对Cu-EDTA的降解特性[J]. 化工学报, 2022, 73(5): 2149-2157.

Hongrui ZHANG, Tian ZHANG, Xizi LONG, Xianning LI. Degradation characteristics of Cu-EDTA by coupling of photocatalysis and microbial fuel cell[J]. CIESC Journal, 2022, 73(5): 2149-2157.

图/表 8

图1 MFC与PEC的串联耦合(a)和并联耦合(b)

Fig.1 Series coupling (a) and parallel coupling (b) of MFC and PEC

图2 TiO2纳米管线LSV图

Fig.2 LSV scan of TiO2 nanotubes

图3 TiO2纳米管的扫描电镜图

Fig.3 SEM images of two different TNAs

图4 MFC装置电极电势及PEC两端电压(a)；耦合系统电流(b)；不同运行条件下系统对Cu-EDTA的去除效果(c)

Fig.4 The electrode potential of the MFC device and the voltage across the PEC (a)； Coupling system current (b)； Removal effect of the system on Cu-EDTA under different operating conditions (c)

图5 单MFC电压及串联MFC输出电压(a)；PEC单元电压及耦合系统电流变化(b)；串联MFC与PEC耦合系统对Cu-EDTA的去除效果(c)

Fig.5 Single MFC voltage and series MFC output voltage (a)； PEC unit voltage and coupling system current change (b)； Cu-EDTA removal effect of series MFC and PEC coupling system (c)

图6 单MFC电压及并联MFC输出电压(a)；PEC单元电压及耦合系统电流变化(b)；并联MFC与PEC耦合系统对Cu-EDTA的去除效果(c)

Fig.6 Single MFC voltage and parallel MFC output voltage (a)； PEC unit voltage and coupling system current change (b)； Parallel MFC and PEC coupling system to remove Cu-EDTA (c)

图7 不同耦合方式系统电流变化(a)；不同耦合方式系统对Cu-EDTA的去除效果(b)；不同耦合方式对Cu离子的去除效果(c)

Fig.7 Current changes in different coupling modes (a)； The removal effect of different coupling modes on Cu-EDTA (b)；The removal effect of different coupling modes on Cu ions (c)

图8 催化电极稳定性测试(a)；氧化基团猝灭实验(b)

Fig.8 Stability test of catalytic electrode (a); Oxidation group quenching experiment (b)

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