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Transcript of regeneration cyclic operation for catalyst life extension ... the optimized reaction/regeneration...

  • 1

    Non-oxidative dehydroaromatization of methane: an effective reaction-

    regeneration cyclic operation for catalyst life extension

    M. Teresa Portilla1, Francisco J. Llopis2, Cristina Martínez1*

    1Instituto de Tecnología Química (UPV-CSIC), Universidad Politécnica de Valencia-Consejo Superior

    de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, Spain. 2Departamento de Ingeniería Química, Universitat de Valencia, 46100 Burjassot, Spain

    * Corresponding author: cmsanche@itq.upv.es; Tel.: (34) 963877811, FAX: (34) 963879444

    Figure S1. X-Ray diffraction (XRD) patterns of (A) ZSM-5, (B) IM-5, (C) TNU-9 and (D) MCM-22 before

    and after the molybdenum loading

    Figure S2. SEM pictures of Mo/ZSM-5 (A1, A2), Mo/IM-5 (B1, B2), Mo/TNU-9 (C1, C2) and

    Mo/MCM-22 (D1, D2), employing a secondary electron (SE) detector (figures on the left), and a

    backscatter electron (BSE) detector (figures on the right). Si and Al are showed in gray scale while

    Mo particles correspond to white dots.

    Figure S3. Methane conversion (A), summatory of yield to HC products (B), selectivity to aliphatics

    (C), to aromatics (D), to benzene (E) and to naphthalene (F) versus time-on-stream over Mo/ZSM-5

    when the carburation step (previous to the reaction) is started at room temperature ( ) or at 723K

    ( )

    Figure S4. Methane conversion (A), total yield to HC products (B) and selectivity to benzene (C) for

    the optimized reaction/regeneration cyclic procedure employing 10 vol.% of O2 in the regeneration

    step and re-carburating the catalyst after the calcination ( ) in comparison with 18h TOS MDA

    reaction ( ) over Mo/IM-5

    Electronic Supplementary Material (ESI) for Catalysis Science & Technology. This journal is © The Royal Society of Chemistry 2015

    mailto:cmsanche@itq.upv.es

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    Figure S5. Methane conversion (A), total yield to HC products (B) and selectivity to benzene (C) for

    the optimized reaction/regeneration cyclic procedure employing 10 vol.% of O2 in the regeneration

    step and re-carburating the catalyst after the calcination ( ) in comparison with 18h TOS MDA

    reaction ( ) over Mo/TNU-9

    Figure S6. Methane conversion (A), total yield to HC products (B) and selectivity to benzene (C) for

    the optimized reaction/regeneration cyclic procedure employing 10 vol.% of O2 in the regeneration

    step and re-carburating the catalyst after the calcination ( ) in comparison with 18h TOS MDA

    reaction ( ) over Mo/MCM-22

  • 3

    Figure S1.

    0 5 10 15 20 25 30 35 40

    2 (degree)

    MCM-22

    Mo/MCM-22

    5 10 15 20 25 30 35 40

    2 (degree)

    TNU-9

    Mo/TNU-9

    0 5 10 15 20 25 30 35 40

    2 (degree)

    IM-5

    Mo/IM-5

    (C) (D)

    (A) (B)

    0 5 10 15 20 25 30 35 40

    2 (degree)

    ZSM-5

    Mo/ZSM-5

  • 4

    Figure S2.

    10 m

    A1 A2

    B1 B2

    C1 C2

    D1 D2

  • 5

    Figure S3.

    0

    4

    8

    12

    16

    20

    0 2 4 6

    CH 4

    Co nv

    er si

    on (%

    )

    TOS (h)

    A

    0

    2

    4

    6

    8

    10

    0 2 4 6

    S Yi

    el d

    to H

    C pr

    od uc

    ts (C

    w t.%

    )

    TOS (h)

    B

    0

    5

    10

    15

    20

    25

    0 2 4 6

    Se le

    ct iv

    ity to

    A lip

    ha tic

    s ( C

    w t.%

    )

    TOS (h)

    C

    75

    80

    85

    90

    95

    100

    0 2 4 6

    Se le

    ct iv

    ity to

    A ro

    m at

    ic s (

    C w

    t.% )

    TOS (h)

    D

    50

    60

    70

    80

    90

    100

    0 2 4 6

    Se le

    ct iv

    ity to

    B en

    ze ne

    (C w

    t.% )

    TOS (h)

    E

    0

    10

    20

    30

    40

    50

    0 2 4 6

    Se le

    ct iv

    ity to

    N ap

    ht ha

    le ne

    (C w

    t.% )

    TOS (h)

    F

  • 6

    Figure S4.

    0

    4

    8

    12

    16

    20

    0 5 10 15 20

    CH 4

    Co nv

    er si

    on (%

    )

    TOS (h)

    A

    0

    2

    4

    6

    8

    10

    0 5 10 15 20 To

    ta lY

    ie ld

    to H

    C (C

    w t.%

    ) TOS (h)

    B

    50

    60

    70

    80

    90

    100

    0 5 10 15 20

    Se le

    ct iv

    ity to

    B en

    ze ne

    (C w

    t.% )

    TOS (h)

    C

  • 7

    Figure S5.

    0

    4

    8

    12

    16

    20

    0 5 10 15 20

    CH 4

    Co nv

    er si

    on (%

    )

    TOS (h)

    A

    0

    2

    4

    6

    8

    10

    0 5 10 15 20 To

    ta l Y

    ie ld

    to H

    C (C

    w t.%

    ) TOS (h)

    B

    50

    60

    70

    80

    90

    100

    0 5 10 15 20

    Se le

    ct iv

    ity to

    B en

    ze ne

    (C w

    t.% )

    TOS (h)

    C

  • 8

    Figure S6.

    0

    4

    8

    12

    16

    20

    0 5 10 15 20

    CH 4

    Co nv

    er si

    on (%

    )

    TOS (h)

    A

    0

    2

    4

    6

    8

    10

    0 5 10 15 20 To

    ta lY

    ie ld

    to H

    C (C

    w t.%

    ) TOS (h)

    B

    50

    60

    70

    80

    90

    100

    0 5 10 15 20

    Se le

    ct iv

    ity to

    B en

    ze ne

    (C w

    t% )

    TOS (h)

    C