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. 2019 Sep 22;24(19):3438. doi: 10.3390/molecules24193438

Table 2.

Works on graphene-based catalysts used in catalytic ozonation.

Catalysts Target Pollutants Reactor Ozonation Conditions Process Performance Reference
GO, oGO, and nOG 4-chlorobenzoic acid
(p-CBA)
C0 = 1 μM
Batch tank reactor.
V = 200 mL
Saturated O3 stock solution (50–60 mg L−1);
O3 dose = 1 mg L−1
pH0 = 3–9
Ccat = 25 mg L−1
p-CBA removal at pH = 9
Ozonation time = 5 min
O3 alone: 60%; O3/nOG: 71%; O3/GO: 78%; O3/oGO: 87%.
[64]
GO, rGO, and nOG 4-chlorobenzoic acid (p-CBA)
C0 = 0.5 μM
Iopromide (IPM)
C0 = 1.0 μM
Batch tank reactor.
V = 200 mL
Saturated O3 stock solution (50–60 mg L−1);
O3 dose = 1 mg L−1 pH0 = 3–7
Ccat = 25 mg L−1
IPM removal at pH = 7
Ozonation time = 5 min
O3 alone: ca. 40%; O3/nOG: ca. 40%;
O3/GO: ca. 90%
[73]
GO, rGO, and g-C3N4 4-chlorobenzoic acid (p-CBA)
Benzotriazole
C0 = 0.084 M
Batch tank reactor
V = 300 mL
CO3 = 2 mg L−1
pH0 = 4.75–6.01
Ccat = 0.5 g L−1
p-CBA removal at pH = 4.75
Ozonation time = 30 min
O3 alone: 87%; O3/GO: 100%; O3/rGO: 100%
[61]
GO N, N-diethyl-m-toluamide (DEET)
C0 = 50 μM
Semi-batch reactor
V = 250 mL
CO3g = 5 mg L−1
Fg = 0.4 L·min−1
pH0 = 2–8
Ccat = 20–100 mg L−1
DEET removal at pH = 7
Ozonation time = 10 min
O3 alone: ca. 40%; O3/GO: 90–95%
[58]
GO and rGO p-hydroxyl benzoic acid (p-HBA)
C0 = 20 mg L−1
Semi-batch reactor
V = 500 mL
CO3g = 20 mg L−1
Fg = 0.1 L·min−1
pH0 = 3.5
Ccat = 0.1 gL−1
p-HBA removal at pH = 3.5
Ozonation time = 30 min
O3 alone: ca. 75%; O3/rGO: 100%
[59]
GO and rGO Oxalic acid
Acetic acid
Formic acid
4-nitrophenol acetylsalicylic acid p-hydroxyl benzoic acid (p-HBA)
C0 = 20 mg L−1
Semi-batch reactor
V = 500 mL
CO3g = 50 mg L−1
Fg = 100 mL min−1
pH0 = 3,
Ccat = 0.1 g L−1
Oxalic acid removal at pH = 3
Ozonation time = 45 min
O3 alone: ca. 10%; O3/rGO: 90–100%
[60]
GO, rGO, N-rGO, S-rGO, and graphene derivative TiO2 composites Oxalic acid
C0 = 90 mgL−1
Semi-batch tank reactor
V = 200 mL
CO3g = 50 mg L−1
Fg = 150 mL min−1
CO3g = 50 mg L−1
pH0 = 3
Ccat = 0.14 g L−1
Oxalic acid removal at pH = 3
Ozonation time = 3 h
O3 alone: ca. 10%; O3/GO: ca. 95%;
O3/rGO: ca. 95%; O3/N-rGO: ca. 95–100%; O3/S-rGO: ca. 95–100%; O3/TiO2-GO: ca. 35–60%; O3/TiO2-rGO: ca. 70–90%
[49]
rGO, N-rGO, and P-rGO Sulfamethoxazole
C0 = 50 mg L−1
Conical flask
V = 100 mL
O3 dosage = 2 g h−1
Fg = 0.4 mL min−1
pH0 = 5–9
Ccat = 1 gL−1
TOC removal at pH = 9
Ozonation time = 20 min
O3 alone: 6%; O3/rGO: 17%; O3/N-rGO:28%; O3/P-rGO: 16%
[67]
rGO and N-rGO 4-nitrophenol
C0 = 50 mgL−1
Semi-batch tank reactor
V = 500 mL
CO3g = 50 mg L−1
Fg = 100 mL min−1
pH0 = 5
Ccat = 0.1 g L−1
TOC removal at pH = 5
Ozonation time = 60 min
O3 alone: ca. 40%; O3/rGO: 80–90%;
O3/N-rGO >95%
[68]
rGO, N-rGO, P-rGO, B-rGO, and S-rGO 4-chlorobenzoic acid (p-CBA)
C0 = 0.084 M
Benzotriazole (BZT)
C0 = 0.084 M
Batch tank reactor
V = 300 mL
CO3 = 2 mg L−1
pH0 = 4.75 (p-CBA)
pH0 = 6.01 (BZT)
Ccat = 0.25 g L−1
p-CBA removal at pH = 4.75.
Ozonation time = 5 min
O3 alone: ca. 40%; O3/rGO: ca. 65%;
O3/S-rGO: ca. 70%; O3/B-rGO: ca. 95%;
O3/P-rGO >95%; O3/N-rGO >95%
[70]
rGO and N-rGO Oxalic acid
C0 = 90 mg L−1
Phenol
C0 = 75 mg L−1
Semi-batch reactor
V = 700 mL
CO3g = 50 mg L−1
Fg = 100 mL min−1
pH0 = 3 (oxalic acid)
pH0 = 8 (phenol)
Ccat = 0.14 g L−1
TOC removal at pH = 8 (phenol oxidation)
Ozonation time = 3 h
O3 alone: ca. 50%; O3/rGO: ca. 60%;
O3/N-rGO: ca. 70–90%
[71]
α-MnO2-rGO Bisphenol A (BPA)
C0 = 4.4 × 10−2 mM
Semi-batch tank reactor
V = 200 mL
CO3g = 50 mg L−1
Fg = 100 mL min−1
pH0 = 3–10
Ccat = 0.1 g L−1
BPA removal at pH = 6.25
Ozonation time = 1 h
O3 alone: 19.1%; O3/α-MnO2-rGO:90.5%
[45]
γ-MnO2-rGO 4-nitrophenol
C0 = 50 mg L−1
Semi-batch tank reactor
V = 1 L
CO3g = 50 mg L−1
Fg = 100 mL min−1
pH0 = 5
Ccat = 0.1 g L−1
TOC removal at pH = 5
Ozonation time = 1 h
O3 alone: ca. 16%; O3/γ-MnO2-rGO:75–85%
[46]
TiO2-GO
Fe3O4-GO
TiO2-Fe3O4-GO
Ibuprofen
C0 = 0.5 µM
Batch tank reactor
V = 1L
CO3,0 = 4 mg·L−1
Ccat = 30 mg L−1
Ibuprofen removal at pH = 7
Ozonation time = 25 min
O3 alone: 55%; O3/GO:76%; O3/Fe3O4-GO:85%
[47]
MnFe2O4-rGO Di-n-butyl phthalate (DBP)
C0 = 0.5 mgL−1
Semi-batch tank reactor
V = 500 mL
Ozone dosage = 0.4 mg min−1
pH0 = 7
Ccat = 10 mg L−1
DBP removal at pH = 7
Ozonation time = 1 h
O3 alone: 32%; O3/MnFe2O4-rGO:87%
[48]

Nomenclature: C0 = initial pollutant concentration; V = working volume; CO3: dissolved ozone concentration; CO3g: ozone gas concentration; Fg: gas flow rate; Ccat: catalyst concentration; pH0 = initial pH; GO = graphene oxide; rGO = reduced graphene oxide; nOG = non-oxidized graphene.