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  • During processing of dairy products, volatile aromacompounds may be lost due to evaporation or thermaldegradation.

    Traditional methods of recovery of aroma compounds:distillation, gas stripping, solvent extraction. But theyinvolve high temperature, high energy consumption orintroduction of other chemicals.

    Pervporation - no damage to aromas, no additives, goodselectivity to aromas.

    Mass transport mechanism: solution-diffusion model

    Pervaporation setup

    Conclusions

    Recovery of aroma compounds from dairy products by pervaporationBoya Zhang1 and Xianshe Feng1, *

    1 Membrane Separation Laboratory, Department of Chemical Engineering, University of Waterloo, Waterloo, ON, Canada N2L 3G1

    Acknowledgements

    Background

    Motivation

    0

    1

    2

    3

    4

    5

    0 500 1000 1500 2000 2500 3000

    Aro

    ma

    flu

    x,

    g/(

    m2.h

    )

    Aroma concentration in feed, ppm

    Nonanal

    Diacetyl

    Hexanoic acid

    Indole

    Dimethyl sulfone

    (b)

    0.1

    1.0

    10.0

    100.0

    1000.0

    10000.0

    2.9 3.0 3.1 3.2 3.3 3.4 3.5

    Perm

    eati

    on

    flu

    x, g

    /(m

    2.h

    )

    1000/T, K-1

    50 500 1000 2500

    Diacetyl concentration in feed, ppm

    } Water

    Diacetyl}

    (a)

    0.1

    1.0

    10.0

    100.0

    Rati

    o o

    f fl

    ux,

    dri

    vin

    g f

    orc

    e o

    r

    perm

    eab

    ilit

    y a

    t 65 ℃

    an

    d 2

    5 ℃

    J65℃/J25℃DF65℃/DF25℃P65℃/P25℃

    0.0

    0.3

    0.6

    0.9

    1.2

    1.5

    0 200 400 600 800 1,000

    Mass

    of

    aro

    ma

    co

    mp

    ou

    nd

    inth

    eo

    rgan

    icp

    hase

    of

    the

    accu

    mu

    late

    dp

    erm

    eate

    ,g

    Operating time, h

    0%

    20%

    40%

    60%

    80%

    100%

    0 100 200 300 400

    Reco

    very

    rate

    of

    dia

    cety

    l

    Operating time, h

    F0/A=226 kg/m2

    F0/A=50 kg/m2

    F0/A=15 kg/m2

    Organophilic membrane

    Investigate the effectiveness of pervaporation on recoveryof aromas from dairy solutions.

    Polymer used as membrane material: PEBA 2533

    Aroma compounds Formula Odor MW (g/mol)

    TB (°C) Solubility in water, 25 °C (g/kg)

    Esters

    Ethyl hexanoate

    Pineapple 144 228 0.46

    Ethyl butanoate

    Pineapple 116 120 5.75

    Ketones

    2-Heptanone

    Banana 114 151 4.3

    Diacetyl

    Buttery 86 88 250

    Acid

    Hexanoic acid

    Goat 116 206 10.82

    Aldehyde

    Nonanal Grass 142 191 0.096

    Sulfur compound

    Dimethyl sulfone

    Hot milk 94 240 Miscible

    Aromatic compound

    Indole

    Jasmine 117 253 1.9

    Characterization of PV performance

    Permeation flux (Ji), g/(m2.h)

    Enrichment factor (β)

    Ni: permeation rate, g/h

    Xi: Aroma concentration in feed, g/g

    Yi: Aroma concentration in permeate, g/g

    𝛽 = 𝑌𝑖/𝑋𝑖

    0

    50

    100

    150

    200

    250

    0 500 1000 1500 2000 2500 3000

    Aro

    ma

    flu

    x,

    g/(

    m2.h

    )

    Aroma concentration in feed, ppm

    2-Heptanone

    Ethyl butanoate

    Ethyl hexanoate

    (a)

    Effect of feed concentration

    0

    5

    10

    15

    20

    25

    30

    0 500 1000 1500 2000 2500 3000

    En

    rich

    men

    tfa

    cto

    r

    Aroma concentration in feed, ppm

    Diacetyl

    Hexanoic acid

    Indole

    Dimethyl sulfone

    (b)

    0

    50

    100

    150

    200

    250

    300

    0 500 1000 1500 2000 2500 3000

    En

    rich

    men

    tfa

    cto

    r

    Aroma concentration in feed, ppm

    Ethyl butanoate

    Ethyl hexanoate

    2-Heptanone

    Nonanal

    (a)

    Effect of temperature

    0

    5

    10

    15

    20

    25

    15 25 35 45 55 65 75

    En

    ric

    hm

    en

    t fa

    cto

    r

    Temperature, ºC

    50 5001000 2500

    Diacetyl concentration in feed, ppm

    Arrhenius-type equation:

    J0: preexponential factor for flux,

    g/(m2.h);

    R: universal gas constant,J/(K.mol); T: absolute temperature, K.

    Reference

    𝑃𝑖 =𝐽 𝑖𝑙𝑖

    𝛾𝑖𝑋𝑖𝑝𝑠𝑎𝑡 −𝑌𝑖𝑝

    𝑝

    𝑙𝑖: membrane thickness, μm𝛾i: activity coefficient 𝑝𝑠𝑎𝑡: saturated pressure, Pa𝑝𝑝: permeate pressure, Pa

    Ca,

    ppm

    Diacetyl-water

    EJa EPa EJw EPw

    50 27.3 -16.4 45.2 1.6

    500 46.6 3.1 43.3 -0.3

    1000 52.0 8.6 42.4 -1.2

    2500 55.0 11.6 43.5 -0.1

    Batch pervaporation

    0%

    20%

    40%

    60%

    80%

    100%

    0 3 6 9 12 15

    Rec

    ove

    ryra

    te

    Operating time, h

    Hexanoic acidDiacetyl

    Ethyl butanoate

    2-Heptanone

    Ethyl hexanoate

    Feng and Huang’s model (well mixed binary feed):

    t: operating time, h;

    F0: initial feed amount, g;

    A: membrane area, m2;

    X0: initial aroma concentration in feed, g/g

    Initial feed amount: 500 g;Initial feed conc.: 320 ppmfor ethyl hexanoate;

    2500 ppm for other aromas;

    Temperature: 36 ℃

    So: aroma solubility in water, g/g;

    Sw: water solubility in aroma, g/g.

    When aroma concentration in accumulated permeate reachesaroma solubility in water, phase separation occurs.

    Ethyl butanoate

    2-Heptanone

    Ethyl hexanoate

    The ratio of initial feed mass (F0) and membrane area (A) affect recovery efficiency.

    To achieve a 100% recovery,

    F0/A = 226 kg/m2, t = 381 h;

    F0/A = 50 kg/m2, t = 84 h;

    F0/A = 15 kg/m2, t =17 h.

    Effect of non-volatile dairy components on PV

    Ethy

    l hex

    anoa

    te

    Nona

    nal

    Ethy

    l buta

    noate

    2-Hep

    tanon

    e

    Hexa

    noic

    acid

    Indole

    Dime

    thyl s

    ulfon

    e

    Diac

    etyl

    0.0

    0.2

    0.4

    0.6

    0.8

    1.0

    1.2

    1.4

    Norm

    aliz

    ed e

    nrichm

    ent

    facto

    r

    NaCl 2 wt% Lactose 2wt%

    Protein 2 wt% Fat 2 wt%

    0 2 4 6 8 10 12 14 16 18 20 22 24 260

    50

    100

    150

    200

    250

    Without non-volatile components

    Whey protein 3.5 wt%

    Fat 3.5 wt%

    NaCl 2 wt%

    Lactose 5 wt%

    To

    tal flu

    x, g

    /(m

    2.h

    )

    Time, h

    1. With an increase in feed aroma concentration ortemperature, aroma fluxes increase rapidly.

    2.The recovery of aroma compound from its aqueous feedsolution is influenced by F0/A for a given period of batchoperating time.

    3. Lactose, whey protein and milk fat in feed negativelyaffect the pervaporative recovery of aroma compounds,due to the hydrophobic interaction between these non-volatile compounds and aromas. NaCl positivelyinfluences the recovery of more hydrophobic aromacompounds.

    Feng, X., Huang, R.Y.M., 1992. Separation of isopropanolfrom water by pervaporation using silicone-basedmembranes. J. Memb. Sci. 74, 171–181.

    Parliment, T.H., McGorrin, R.J., 2000. Critical flavorcompounds in dairy products, in: Flavor Chemistry:Industrial and Academic Research. American ChemicalSociety, Washington, D.C., pp. 44–71.

    0 2 4 6 8 10 12 14 16 18 20 22 24 260

    40

    80

    120

    160

    200

    240

    Enri

    chm

    ent fa

    cto

    r of eth

    yl buta

    no

    ate

    Time, h

    In general, lactose,

    whey protein or milk fat

    in feed solutions

    negatively affected the

    pervaporative recovery

    of aroma compounds.

    NaCl positively

    influenced the recovery

    of more hydrophobic

    aroma compounds.

    No concentration polarization or membrane fouling with the

    presence of lactose, whey protein, fat and NaCl was observed.


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