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Solar Photocatalysis for Urban and Industrial Waste Water Reclamation. Sixto Malato Plataforma Solar de Almería (PSA-CIEMAT ), Tabernas (Almería), Spain . 1. 5. 6. 1. Central receiver technology. 2. Parabolic dishes + Stirling engines. 4.

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solar photocatalysis for urban and industrial waste water reclamation
Solar Photocatalysis for Urban and Industrial Waste Water Reclamation

Sixto Malato

Plataforma Solar de Almería (PSA-CIEMAT),

Tabernas (Almería), Spain.

slide2

1

5

6

1. Central receiver technology

2. Parabolic dishes + Stirling engines

4

3. Parabolic-trough technology (thermal oil)

4. Parabolic-trough technology (DSG)

1

5. Parabolic-troughs (gas) + Molten Salt TES

6. Linear Fresnel Collector

7

9

7. Solar furnaces

2

8

8. Water desalination

3

9. Water photocatalysis

10. Passive architecture

10

slide3

Introduction

Solar AdvancedOxidationProcesses

“near ambient temperature and pressure water treatment processes driven by solar energywhich involve the generation

of hydroxyl radicals in sufficient quantity

to effective water purification”

driven by solar energy

1/38

slide4

Introduction

Wavelength, µm

2/38

slide5

Introduction

CATALYSIS

+

SUN

3/38

slide7

Introduction

1 Sun CPCs

  • Turbulent flow conditions
  • No vaporization of volatile compounds
  • No solar tracking
  • No overheating
  • Direct and Diffuse radiation
  • Low cost
  • Weatherproof (no contamination)

5/38

slide9

Introduction

The current lack of data for comparison of solar photocatalysis with other technologies definitely presents an obstacle towards an industrial application. Therefore, it is necessary:

  • Give sound examples of techno-economic studies.
  • Assessment of the environmental impact: life cycle analysis (LCA).
  • To lead to industry application it will be critical that the processes can be developed up to a stage, where the process:
  • can be compared to other processes.
  • is robust, i.e. small to moderate changes to the wastewater stream do not affect the plant’s efficiency and operability strongly.
  • is predictable, i.e. process design and up-scaling can be done reliably.
  • gives additional benefit to the industry applying the process (e.g. giving the company the image of being “green”).

7/38

slide10

Examples of techno-economicstudies

Sound examples of techno-economic studies:

AOP-BIO and BIO-AOP

Lanfill leachate

Treatment of Ecs

Combination NF/AOPs

8/38

slide12

AOP

EVALUATION OF BIODEGRADABILITY DURING AOP

AOP-BIO and BIO-AOP

WW characterization: TOC, COD, BOD, main inorganics, contaminants (LC-MS/GC-MS)

TOXICITY

Non-toxic or partially toxic (<50%)

Toxic (>50%)

EVALUATION OF

BIODEGRADABILITY

2

1

1

TOC>500 mg/L

TOC<500 mg/L

DILUTION AND EVALUATION OF BIODEGRADABILITY

2

EVALUATION OF BIODEGRADABILITY DURING AOP

AOP

2

1

1

BIOLOGICAL

TREATMENT

2

EVALUATION OF BIODEGRADABILITY DURING AOP

BIOLOGICAL

TREATMENT

AOP

BIOLOGICAL

TREATMENT

1

2

COD and toxicity<Guideline

DISCHARGE

Biorecalcitrant compounds

COD and toxicity<Guideline

DISCHARGE

AOP

2: Biodegradable. COD>Guideline

1: Partially or not biodegradable

10/38

slide13

Non-biodegradable pesticides

Biodegradable compounds

AOP-BIO

Combined photo-Fenton and biotreatment

Industrial wastewater

DOC0: 480 mg/L

Decontaminated water

DOC: 75 mg/L

Biological treatment (IBR)

Solar Photo-Fenton

  • 20 mg/L Fe / pH: 2.8
  • 44 % mineralization
  • DOCf: 270 mg/L
  • 21 mM H2O2 consumed
  • DOC0: 300 mg/L
  • 1.5 days of biotreatment
  • 75 % mineralization
  • DOCresidual: 75 mg/L

11/38

slide14

AOP-BIO

1. SPE extraction

1

2

3

4

2. LC-TOF-MS

Oasis®HLB

  • Concentration of all pesticides decreased gradually throughout the process (mainly during the photo-Fenton process).
  • After the combined system: totally removed, except pyrimethanil and thiacloprid, found in range of g/L

12/38

slide15

BIO-AOP

Real WW

13/38

slide16

BIO-AOP

INITIAL CONDITIONS (photo-Fenton)

  • Nalidixicacid: 39 mg/L
  • Initial TOC: 822 mg/L
  • [NaCl] : 6.5 g/L
  • Total degradation of the nalidixic acid

at 350 minutes (illumination time)

(65 mM H2O2)

  • 28% of the initial TOC was removed

14/38

slide17

100

80

60

% TOC reduction

40

20

0

AOP-BIO and BIO-AOP

t30w = 21 min (elim. NXA) !!!

H2O2 = 12 mM (elim. NXA) !!!

Biotr. time = 4 days

Biotr. time = 4 days

AOP BIO

BIO  AOP

t30w= 350 min; H2O2 = 65 mM

(elim.NXA)

15/38

slide18

No DPs

BIO-AOP

LC-TOF-MS chromatograms

Retention time (min)

16/38

slide19

2. Photo-Fenton (Fe 1 mM)

3. Evaluation of toxicity

and biodegradability

3.a Respirometryactivatedsludge

3.b BiodegradabilitybyZahn-Wellens

Landfillleachate

Landfillleachate (COD: 15615 mg/L; DQO: 42630 mg/L)

  • Pre-treatment

(Coagulation/floculation)

17/38

slide20

Landfillleachate

Respirometryactivatedsludge

18/38

slide21

Landfillleachate

BiodegradabilitybyZahn-Wellens

19/38

slide22

Landfillleachate

  • Pre-treatment (Coagulation/floculation)

2. PHOTO-FENTON

(<20 % mineralization)

3. BIOTREATMENT

20/38

slide23

Treatment of ECs

WWTPs

NATURAL WATERS

(ng-μg/L)

EMERGING CONTAMINANTS

  • Untilrecentlyunknown
  • Commonly use
  • Emergingrisks (EDCs, antibiotics)
  • Unregulated

INCOMPLETE

REMOVAL

Photochemicaltransformations

CONTINUOUS INTRODUCTION

INTO THE ENVIRONMENT

TRANSFORMATION

PRODUCTS

21/38

slide25

Treatment of ECs

LC-QLIT-MS/MS

CHARACTERIZATION

29/62 Compoundswithhighercontribution in MWTP Effluent

23/38

slide26

Treatment of ECs

75 L, 4.1 m2, control T (35 ºC)

50 L, 0.69 g O3 h-1

24/38

slide27

Ozonation

Treatment of ECs

Solar TiO2.

Solar photo-Fenton

1-Bisphenol A; 2-Ibuprofen; 3-Hydrochlorothiazide;

4-Diuron; 5-Atenolol; 6-4-AA;

7-Diclofenac; 8-Ofloxacin; 9-Trimethoprim;

10-Gemfibrozil; 11-4-MAA; 12-Naproxen;

13-4-FAA; 14-∑C; 15-4-AAA; 16-Caffeine; 17-Paraxanthine

Contaminants > 1000 ngL-1.

∑C = rest of contaminants

at less than 1000 ngL-1

25/38

slide28

Treatment of ECs

Toxicity assays during ozonation and photo-Fenton showed < 10% inhibition on V. fisheri bioluminescence and in respirometric assays with municipal activated sludge

LC-MS chromatogram. Ozonation.

t = 0

t = 60 min

LC-MS chromatogram. Photo-Fenton.

t = 0

t = 20 (t30W = 14) min

26/38

slide29

Treatment of ECs

Calculation basis:

90% or 98% degradation

of micropollutants 5000 m3/day

H2O2 1.1 € kg-1

Fe(II) 0.72 € kg-1

H2SO4 0.20 € kg-1

NaOH 0.12 € Kg-1

Electricity 0.07 € Kwh-1

O20.15 € Kg-1

Labour18.8 € h-1

23.1 € kg O3

27/38

slide31

Combination NF/AOPs

NF in parallel (5.2 m2).

1.4 m3h-1

29/38

slide32

Combination NF/AOPs

Micropollutants

at 15 µg L-1, each

30/38

slide33

Combination NF/AOPs

Solar photocatalysis

31/38

slide34

Combination NF/AOPs

r = kC

Fe (II), 0.1 mM

H2O2, 25 mg L-1

Natural pH

32/38

slide35

Combination NF/AOPs

Fe (II), 0.1 mM

0.2 mMEDDS

H2O2, 25 mg L-1

Natural pH

Fe(III)-L + hν → [Fe(III)-L]* → Fe(II) + L•

Ethylenediamine-N,N'-disuccinicacid (EDDS)

33/38

slide36

Combination NF/AOPs

Operational requirements for attaining 95% of pharmaceuticals degradation present in NF concentrates (CF=4 and 10) when solar photo-Fenton and photo-Fenton like Fe(III)-EDDS complex were applied. CF=1, no NF, only AOP.

34/38

slide37

Heterogeneousphotocatalytichydrogen

generation in a solar pilotplant

Flow rate 20 L/min.

CPC with pyrexglass tubes, 1.375 m2.

Irradiated volume 9.79 L.

Total volume 25 L.

Catalyst loading 0.2-1 g/L, Pt/(TiO2-N) or Pt/(CdS-ZnS)

Sacrificial agents:

formic acid (0.05 M), glycerol (0.001 M)

and a municipal wastewater (97.7 mg/L of DOC).

35/38

slide38

Heterogeneousphotocatalytichydrogen

generation in a solar pilotplant

36/38

slide39

Heterogeneousphotocatalytichydrogen

generation in a solar pilotplant

0.05 M formic acid

Real wastewater, 98 mg/L of DOC

Reaction conditions: 5 g of catalyst, 25 L of aqueous solution. Data corresponding to 5 hours of irradiation.

K. Villa, X. Domènech, S. Malato, M. I. Maldonado, J. Peral.

Heterogeneousphotocatalytichydrogengeneration in a solar pilotplant.

Int. J. HydrogenEnergy, 38 (29), 2013, 12718-12724.

37/38

slide40

Acknowledgements

Unidad de Tratamientos Solares de Agua (Solar Treatment of Water Research Group) .

Plataforma Solar de Almería (CIEMAT).

38/38