CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case

Emil Sebastian Gutterød; Sigurd Øien-ødegaard; Koen Bossers; Anne-eva Nieuwelink; Maela Manzoli; Luca Braglia; Andrea Lazzarini; Elisa Borfecchia; Sajjad Ahmadigoltapeh; Boris Bouchevreau; Bjørn Tore Lønstad-bleken; Reynald Henry; Carlo Lamberti; Silvia Bordiga; Bert M. Weckhuysen; Karl Petter Lillerud; Unni Olsbye

doi:10.1021/acs.iecr.7b01457

CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case

Emil Sebastian Gutterød, Sigurd Øien-ødegaard, Koen Bossers, Anne-eva Nieuwelink, Maela Manzoli, Luca Braglia, Andrea Lazzarini, Elisa Borfecchia, Sajjad Ahmadigoltapeh, Boris Bouchevreau, Bjørn Tore Lønstad-bleken, Reynald Henry, Carlo Lamberti, Silvia Bordiga, Bert M. Weckhuysen, Karl Petter Lillerud, Unni Olsbye

Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, Sem Saelandsvei 26, N-0315 Oslo, Norway
Department of Chemistry, NIS Interdepartmental Centre and INSRM reference centre, University of Turin, via Quarello 15A, I-10135 Turin, Italy
IRC “Smart Materials”, Southern Federal University, Zorge Street 5, 344090 Rostov-on-Don, Russia

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220–280 °C and ambient pressure, with H2/CO2 = 0.2–9 and contact times, τ = 0.004–0.01 gcat×min×ml−1. The catalysts were characterized by XRD, N2 adsorption, FESEM, TEM and HRTEM, dissolution-NMR, CO chemisorption, IR spectroscopy and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 micron crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with Eapp = 50±3 kJ×mol−1. However, the turn-over frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 hours testing.

Original language	English
Pages (from-to)	13206-13218
Journal	Industrial & Engineering Chemistry Research
Volume	56
Issue number	45
DOIs	https://doi.org/10.1021/acs.iecr.7b01457
Publication status	Published - 15 Nov 2017

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acs.iecr.7b01457Final published version, 2.41 MBLicence: Taverne

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Gutterød, E. S., Øien-ødegaard, S., Bossers, K., Nieuwelink, A., Manzoli, M., Braglia, L., Lazzarini, A., Borfecchia, E., Ahmadigoltapeh, S., Bouchevreau, B., Lønstad-bleken, B. T., Henry, R., Lamberti, C., Bordiga, S., Weckhuysen, B. M., Lillerud, K. P., & Olsbye, U. (2017). CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case. Industrial & Engineering Chemistry Research, 56(45), 13206-13218. https://doi.org/10.1021/acs.iecr.7b01457

@article{ad2e0c0841994a6c83d2db89a31e876c,

title = "CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case",

abstract = "CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220–280 °C and ambient pressure, with H2/CO2 = 0.2–9 and contact times, τ = 0.004–0.01 gcat×min×ml−1. The catalysts were characterized by XRD, N2 adsorption, FESEM, TEM and HRTEM, dissolution-NMR, CO chemisorption, IR spectroscopy and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 micron crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with Eapp = 50±3 kJ×mol−1. However, the turn-over frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 hours testing. ",

author = "Gutter{\o}d, \{Emil Sebastian\} and Sigurd {\O}ien-{\o}degaard and Koen Bossers and Anne-eva Nieuwelink and Maela Manzoli and Luca Braglia and Andrea Lazzarini and Elisa Borfecchia and Sajjad Ahmadigoltapeh and Boris Bouchevreau and L{\o}nstad-bleken, \{Bj{\o}rn Tore\} and Reynald Henry and Carlo Lamberti and Silvia Bordiga and Weckhuysen, \{Bert M.\} and Lillerud, \{Karl Petter\} and Unni Olsbye",

year = "2017",

month = nov,

day = "15",

doi = "10.1021/acs.iecr.7b01457",

language = "English",

volume = "56",

pages = "13206--13218",

journal = "Industrial \& Engineering Chemistry Research",

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Gutterød, ES, Øien-ødegaard, S, Bossers, K, Nieuwelink, A, Manzoli, M, Braglia, L, Lazzarini, A, Borfecchia, E, Ahmadigoltapeh, S, Bouchevreau, B, Lønstad-bleken, BT, Henry, R, Lamberti, C, Bordiga, S, Weckhuysen, BM, Lillerud, KP & Olsbye, U 2017, 'CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case', Industrial & Engineering Chemistry Research, vol. 56, no. 45, pp. 13206-13218. https://doi.org/10.1021/acs.iecr.7b01457

TY - JOUR

T1 - CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case

AU - Gutterød, Emil Sebastian

AU - Øien-ødegaard, Sigurd

AU - Bossers, Koen

AU - Nieuwelink, Anne-eva

AU - Manzoli, Maela

AU - Braglia, Luca

AU - Lazzarini, Andrea

AU - Borfecchia, Elisa

AU - Ahmadigoltapeh, Sajjad

AU - Bouchevreau, Boris

AU - Lønstad-bleken, Bjørn Tore

AU - Henry, Reynald

AU - Lamberti, Carlo

AU - Bordiga, Silvia

AU - Weckhuysen, Bert M.

AU - Lillerud, Karl Petter

AU - Olsbye, Unni

PY - 2017/11/15

Y1 - 2017/11/15

N2 - CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220–280 °C and ambient pressure, with H2/CO2 = 0.2–9 and contact times, τ = 0.004–0.01 gcat×min×ml−1. The catalysts were characterized by XRD, N2 adsorption, FESEM, TEM and HRTEM, dissolution-NMR, CO chemisorption, IR spectroscopy and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 micron crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with Eapp = 50±3 kJ×mol−1. However, the turn-over frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 hours testing.

AB - CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220–280 °C and ambient pressure, with H2/CO2 = 0.2–9 and contact times, τ = 0.004–0.01 gcat×min×ml−1. The catalysts were characterized by XRD, N2 adsorption, FESEM, TEM and HRTEM, dissolution-NMR, CO chemisorption, IR spectroscopy and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 micron crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with Eapp = 50±3 kJ×mol−1. However, the turn-over frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 hours testing.

U2 - 10.1021/acs.iecr.7b01457

DO - 10.1021/acs.iecr.7b01457

M3 - Article

SN - 0888-5885

VL - 56

SP - 13206

EP - 13218

JO - Industrial & Engineering Chemistry Research

JF - Industrial & Engineering Chemistry Research

IS - 45

ER -

CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs—The Base Case

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