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Progress in Chemistry 2019, Vol. 31 Issue (8): 1187-1198 DOI: 10.7536/PC190139 Previous Articles   

Complexed Heavy Metal Wastewater Treatment: Decomplexation Mechanisms Based on Advanced Oxidation Processes

Shiying Yang1,2,3,**(), Yichao Xue3, Manqian Wang3   

  1. 1. The Key Laboratory of Marine Environment & Ecology of Ministry of Education, Qingdao 266100,China
    2. Shandong Provincial Key Laboratory of Marine Environment and Geological Engineering(MEGE), Qingdao 266100,China
    3. College of Environmental Science and Engineering, Ocean University of China, Qingdao 266100, China
  • Received: Online: Published:
  • Contact: Shiying Yang
  • About author:
    ** E-mail:
  • Supported by:
    National Natural Science Foundation of China(21677135)
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Due to the presence of strong ligands such as ethylenediaminetetraacetic acid (EDTA), complexed heavy metals have high stability and complex morphology, and are difficult to be removed from wastewater by conventional water treatment methods such as adsorption, ion exchange, membrane separation, etc. Advanced oxidation technology(AOPs) is the first choice for the removal of heavy metals in complex state due to its strong oxidizing properties. It can not only decompose heavy metals, but also degrade the ligands. In the publishing research, the mechanisms of decomplexing using AOPs include the following aspects: (1) strong oxidation of free radicals, (2) gradual decarboxylation of ligands with EDTA, (3) self-catalysis of variable valence metal ions, (4) intermetallic substitution, (5) electrolysis, (6) multiple mechanisms combined, such as simultaneous decomplexation, mineralization of ligands, and recovery of heavy metals. In this review, from the perspective of different metals and ligands and their ability to complex, the research development of complexed heavy metal wastewater treatment are summarized, and the different complexation mechanisms based on AOPs are discussed. At the same time, the problems worthy of in-depth study are prospected.

Key words: heavy metal complex, decomplexation, advanced oxidation processes, Fenton technology, stepwise decarboxylation, replacement
Fig. 1 Web of Science data analysis of(complexed) heavy metal removal studies
Table 1 Typical case study on removing heavy metal complex based on advanced oxidation processes
Decomplexation mechanism Complex AOPs Typical condition Removal
efficiency		 ref
·OH
oxidation		 Cu/Ni-EDTA E-Fenton Current density=20 mA/cm2, [H2O2]0=6 mL·L-1·h-1, pH=2.0 Standard discharge 22
Ni-EDTA Fenton [H2O2]0=141 mM, [Fe2+]0=1.0 mM,[Fe3 +]0=1.0 mM, pH=3.0,
T=25~50 ℃		 Ni > 92% 25
Fenton + US [H2O2]0=141 mM, [Fe2+]0=1.0 mM, pH=3.0, t=60 min Ni:95.3% 30
Advanced-Fenton [H2O2]0 =35.2 mM, [Fe0]0 =4.0 g·L-1, pH=2.5 Ni:98.4% 31
Fenton + O3 [H2O2]0=1.0 mL·L-1, [Fe2+]0=150 mg·L-1, [Fe2+]0/[H2O2]0
=1.46, [O3]0=252 mg L-1, pH=3.0		 Ni:99.84%,
TOC:57.13%		 78
Stepwise decarboxylation Cu-EDTA Discharge Plasma Discharge voltage=19 kV, t=60 min Cu-EDTA:99.7% 23
O3 [Fe2+]0=1.0 mM, pH=3.0, [O3]0=30 mg·min-1·L-1, [Cu2+]=
64 mg·L-1		 TOC:75%~80%
Cu:90%~97%		 73
Photo-electrocatalytic Current density=1.13 A/m2, pH=3.5, t=60 min Cu-EDTA:80% 80
Photo-electrocatalytic Current density=0.5 mA/cm2, Rotation speed=100 rpm, pH=3.18 Cu-EDTA:74.18% 90
Fe(Ⅲ)
displacement		 Cr-organic FeS + H2O2 [H2O2]0=20 mM,[FeS]0=4.0 g·L-1,pH=3.0 Cr < 0.3 mg/L 4
Cu-EDTA Fe(Ⅲ)/UV/OH [Fe]/[Cu]=9∶1, t=6 min, pH=1.5~3.0 Cu-EDTA > 95% 10
Cu-organic Fe(Ⅲ)/UV/OH [Fe]/[Cu]=4∶1, t=10 min, pH=1.8~5.4 Cu:99.8%;TOC:30%~48% 24
Cr-organic UV/Fe(Ⅲ) [Fe3+]0=0.8 mM,pH=2.5~3.0, t=30 min Cr < 0.36 mg/L;TOC:60% 26
Self-catalytic Cu-EDTA UV/H2O2 / Cu-EDTA:82.2% 87
Photo-Fenton [AA]: [Cu-EDTA]=1,UV dose:1.25×105 J/m2 ,pH=2.0 Cu:77.6% 97
UV/Chlorine Rm ([NaClO]0 / [Cu]0)=10, pH=11.0 Cu-EDTA:~70% 98
Electrolysis Cu-EDTA Micro-electrolysis [Fe2+]=374.0 mg·L-1, pH=2.0~2.3, t=5 min Cu:100% 99
Fe:C=2, pH=3.0, t=40 min TOC:32.3%; Cu:98.2% 101
Fe:C=0.02, pH=2.0, T=25 ℃, t=60 min TOC:200 mg/L→40.66 mg/L;
Cu:60 mg/L→1.718 mg/L		 102
Ni-EDTA Iron scraps packed-bed anode Current=0.5 A,pH=3,Air-purged rate=0.2 L·min-1, T=313 K,
t=30 min		 TOC:95.8%
Ni:94.3%		 104
Ni-ammonia Electro-oxidation Current density=32 mA/cm2, pH=9.0, T=60 ℃ Ni:99%, NH3:70% 107
Fig. 2 Enhanced self-catalytic pathway of Cu-EDTA degradation with H2O2/UV[96]
Fig. 3 Schematic diagram of the Fe(Ⅲ)/UV/OH process[24]
Fig. 4 Plausible pathways for treatment of Cr(Ⅲ)-citrate complex by pyrite/H2O2[4]
Fig. 5 Photoelectrocatalytic decomposition of copper-cyanide in the presence of EDTA/K4P2O7[90]
Fig. 6 Summary of the principle of removing complexed heavy metals based on advanced oxidation processes
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