presentation march
TRANSCRIPT
Ozonation catalysed by Me/support catalysts.
Liudmyla Masliuk
11.03.2014
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 1 / 15
Introduction
Does the catalyst decompose ozone?
Is ozonation with catalyst more efficient than without?
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 2 / 15
Various catalysts
Article Effective catalysts for decomposition of aqueous ozoneAuthors Jianjun Lin , Akimasa Kawai, Tsuyoshi NakajimaJournal Applied Catalysis B: Environmental 39 (2002) 157 − 165
Catalyst Pt, Pd, Ag, Ru, Rh, Ir, Ni, Cd, Mn, Fe, Cu, Zn, Zr, Co, Y,Mo, Ti and Au
Support AC, zeolite (HY and mordenite), Al2O3, SiO2 ,SiO2 · Al2O3 and TiO2
Preparation impregnationPollutant no
Details Al2O3 stable against ozone, Pt/SiO2 gives best rateResult 3% Pd/SiO2 the most effective
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 3 / 15
Few more details
CatalystsSupport, impregnated torespective salt solution wasdried for 1 night at 383 K andthan calcined for 3 h at 773 K
OzoneWater, saturated with ozonewas pumped through a catalyticbed and ozone level wasmeasured before and afterflowing through.
SupportsOzone decomposition rate forsome supports
Support Rate (mgO3min−1g−1
cat )AC 0.25
Zeolite (mordenite) 0.02Al2O3, SiO2 0.01
others 0
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 4 / 15
Few more details
CatalystsSupport, impregnated torespective salt solution wasdried for 1 night at 383 K andthan calcined for 3 h at 773 K
OzoneWater, saturated with ozonewas pumped through a catalyticbed and ozone level wasmeasured before and afterflowing through.
SupportsOzone decomposition rate forsome supports
Support Rate (mgO3min−1g−1
cat )AC 0.25
Zeolite (mordenite) 0.02Al2O3, SiO2 0.01
others 0
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 4 / 15
Few more details
CatalystsSupport, impregnated torespective salt solution wasdried for 1 night at 383 K andthan calcined for 3 h at 773 K
OzoneWater, saturated with ozonewas pumped through a catalyticbed and ozone level wasmeasured before and afterflowing through.
SupportsOzone decomposition rate forsome supports
Support Rate (mgO3min−1g−1
cat )AC 0.25
Zeolite (mordenite) 0.02Al2O3, SiO2 0.01
others 0
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 4 / 15
Main results
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 5 / 15
Pd and Pt
SurfaceCatalyst Specific surface Rate,
area, m2/g mgO3/min/gcat
Pd/SiO2 206 0.77Pd/SiO2 · Al2O3 221 0.54
Pd/Al2O3 139 0.39Pd/TiO2 34 0.35
AmountCatalyst Amount, Rate,
% mgO3/min/gcat
Pd/SiO2 0.5 0.681 0.843 0.965 0.77
Pd/Al2O3 0.5 0.421 0.463 0.505 0.40
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 6 / 15
Pd and Pt
SurfaceCatalyst Specific surface Rate,
area, m2/g mgO3/min/gcat
Pd/SiO2 206 0.77Pd/SiO2 · Al2O3 221 0.54
Pd/Al2O3 139 0.39Pd/TiO2 34 0.35
AmountCatalyst Amount, Rate,
% mgO3/min/gcat
Pd/SiO2 0.5 0.681 0.843 0.965 0.77
Pd/Al2O3 0.5 0.421 0.463 0.505 0.40
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 6 / 15
Pd and Pt
SurfaceCatalyst Specific surface Rate,
area, m2/g mgO3/min/gcat
Pd/SiO2 206 0.77Pd/SiO2 · Al2O3 221 0.54
Pd/Al2O3 139 0.39Pd/TiO2 34 0.35
AmountCatalyst Amount, Rate,
% mgO3/min/gcat
Pd/SiO2 0.5 0.681 0.843 0.965 0.77
Pd/Al2O3 0.5 0.421 0.463 0.505 0.40
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 6 / 15
Ru/CeO2
Article Relationship between the structure of Ru/CeO2 catalystsand their activity in the catalytic ozonation of succinic acidaqueous solutions
Authors F. Delanoe, B. Acedo, N. Karpel Vel Leitner, B. LegubeJournal Applied Catalysis B: Environmental 29 (2001) 315 − 325
Preparation impregnation or acid exchangePollutant succinic acid
Result impregnated catalyst gives better efficiency
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 7 / 15
Preparation
2% Ru/CeO2
ImpregnationSupport impregnated intoRu(NH3)6Cl3 solution for 20 h,dried at 323K, than reducedunder hydrogen flow for 20 h at623K≥ 1.4%Ru
Acid exchangeRuCl3 solution at pH 2.4 in HClwas stirred with CeO2 powderfor 20h and treated in the sameway after filtration and drying≥ 1.1%Ru
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 8 / 15
Preparation
2% Ru/CeO2
ImpregnationSupport impregnated intoRu(NH3)6Cl3 solution for 20 h,dried at 323K, than reducedunder hydrogen flow for 20 h at623K≥ 1.4%Ru
Acid exchangeRuCl3 solution at pH 2.4 in HClwas stirred with CeO2 powderfor 20h and treated in the sameway after filtration and drying≥ 1.1%Ru
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 8 / 15
Procedure
O3 was introduced continuously to aqueous solution of succinicacid in a presence of powdered catalyst2 sets of conditions: SA 1 mmol/l , catalyst 0.8 g/l and SA 5mmol/l , catalyst 3.2 g/l4 experiments: 0.5 mmol/l SA for impregnated and 0.3 mmol/lfor acid exchanged catalystSA removed by ozonation at this conditions (pH = 3.4) < 4%SA absorbed < 10%
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 9 / 15
Concentration
Low concentration High concentration
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 10 / 15
Multiple treatment
Initial rates of SA (�) and TOC (�) conversion for four successivecatalytic ozonation experiments; Fig. a: I catalyst; Fig. b: AE catalyst.
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 11 / 15
Ru/CeO2
Article Catalytic ozonation of chlorinated carboxylic acids withRu/CeO2 − TiO2 catalyst in the aqueous system
Authors Hongxiang Fu, Nathalie Karpel Vel Leitner and BernardLegube
Journal New J. Chem., 2002, 26, 1662 − 1666Preparation impregnation or acid exchange
Pollutant Chloroacetic acid (CAA) and chlorosuccinic acid (CSA)
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 12 / 15
CAA. pH control
Room temperature, catalyst amount: 0.8 gL−1, introduced O3 flowrate: 1275 ± 25 mgh−1
pH influence
pKa of CAA 2.86. CAA initialconcentration: 0.65 mM.
pH adjustment
Initial pH: 3.1, CAA initialconcentration: 2.0 mM.
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 13 / 15
CAA. pH control
Room temperature, catalyst amount: 0.8 gL−1, introduced O3 flowrate: 1275 ± 25 mgh−1
pH influence
pKa of CAA 2.86. CAA initialconcentration: 0.65 mM.
pH adjustment
Initial pH: 3.1, CAA initialconcentration: 2.0 mM.
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 13 / 15
Ru/Al2O3 + Ce
Catalytic activity of cerium-doped Ru/Al2O3 during ozonation ofdimethyl phthalateYunrui ZHOU, Wanpeng ZHU, Xun CHEN Sci. Engin. China 2008,2(3): 354 − 357
TOC removal ratecatalyst Chet CO Chom CabsRu-Ce 35.4 24.1 33.1 7.40Ce-Ru 42.6 24.9 24.8 7.65
mixture of Ce and Ru 45.8 26.4 19.7 8.10Ru 50.4 38.0 − 11.6
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 14 / 15
Ce amount influence
Ce load
Ce ions influence
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 15 / 15
Ce amount influence
Ce load Ce ions influence
Liudmyla Masliuk (SERP-Chem M2) Ozonation catalysed by Me/support catalysts. 11.03.2014 15 / 15