Intermetallic GaPd2 Nanoparticles on SiO2 for Low-Pressure CO2 Hydrogenation to Methanol: Catalytic Performance and In Situ Characterization

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

A nanodispersed intermetallic GaPd2/SiO2 catalyst is prepared by simple impregnation of industrially relevant high-surface-area SiO2 with Pd and Ga nitrates, followed by drying, calcination, and reduction in hydrogen. The catalyst is tested for CO2 hydrogenation to methanol at ambient pressure, revealing that the intrinsic activity of the GaPd2/SiO2 is higher than that of the conventional Cu/ZnO/Al2O3, while the production of the undesired CO is lower. A combination of complementary in situ and ex situ techniques are used to investigate the GaPd2/SiO2 catalyst. In situ X-ray diffraction and in situ extended X-ray absorption fine structure spectroscopy show that the GaPd2 intermetallic phase is formed upon activation of the catalyst via reduction and remains stable during CO2 hydrogenation. Identical location-transmission electron microscopy images acquired ex situ (i.e., micrographs of exactly the same catalyst area recorded at the different steps of activation and reaction procedure) show that nanoparticle size and dispersion are defined upon calcination with no significant changes observed after reduction and methanol synthesis. Similar conclusions can be drawn from electron diffraction patterns and images acquired using environmental TEM (ETEM), indicating that ETEM results are representative for the catalyst treated at ambient pressure. The chemical composition and the crystalline structure of the nanoparticles are identified by scanning TEM energy dispersive X-ray spectroscopy, selected area electron diffraction, and atomically resolved TEM images.
Original languageEnglish
JournalA C S Catalysis
Volume5
Issue number10
Pages (from-to)5827-5836
Number of pages10
ISSN2155-5435
DOIs
Publication statusPublished - 2015

Keywords

  • Methanol synthesis
  • Intermetallics
  • In situ characterization
  • XRD
  • TEM
  • EXAFS

Cite this

@article{9e65d38cb8ef4cf892b5a66193946aa4,
title = "Intermetallic GaPd2 Nanoparticles on SiO2 for Low-Pressure CO2 Hydrogenation to Methanol: Catalytic Performance and In Situ Characterization",
abstract = "A nanodispersed intermetallic GaPd2/SiO2 catalyst is prepared by simple impregnation of industrially relevant high-surface-area SiO2 with Pd and Ga nitrates, followed by drying, calcination, and reduction in hydrogen. The catalyst is tested for CO2 hydrogenation to methanol at ambient pressure, revealing that the intrinsic activity of the GaPd2/SiO2 is higher than that of the conventional Cu/ZnO/Al2O3, while the production of the undesired CO is lower. A combination of complementary in situ and ex situ techniques are used to investigate the GaPd2/SiO2 catalyst. In situ X-ray diffraction and in situ extended X-ray absorption fine structure spectroscopy show that the GaPd2 intermetallic phase is formed upon activation of the catalyst via reduction and remains stable during CO2 hydrogenation. Identical location-transmission electron microscopy images acquired ex situ (i.e., micrographs of exactly the same catalyst area recorded at the different steps of activation and reaction procedure) show that nanoparticle size and dispersion are defined upon calcination with no significant changes observed after reduction and methanol synthesis. Similar conclusions can be drawn from electron diffraction patterns and images acquired using environmental TEM (ETEM), indicating that ETEM results are representative for the catalyst treated at ambient pressure. The chemical composition and the crystalline structure of the nanoparticles are identified by scanning TEM energy dispersive X-ray spectroscopy, selected area electron diffraction, and atomically resolved TEM images.",
keywords = "Methanol synthesis, Intermetallics, In situ characterization, XRD, TEM, EXAFS",
author = "Fiordaliso, {Elisabetta Maria} and Irek Sharafutdinov and Carvalho, {Hudson W. P.} and Jan-D. Grunwaldt and Hansen, {Thomas Willum} and Ib Chorkendorff and Wagner, {Jakob Birkedal} and Damsgaard, {Christian Danvad}",
year = "2015",
doi = "10.1021/acscatal.5b01271",
language = "English",
volume = "5",
pages = "5827--5836",
journal = "A C S Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "10",

}

Intermetallic GaPd2 Nanoparticles on SiO2 for Low-Pressure CO2 Hydrogenation to Methanol : Catalytic Performance and In Situ Characterization. / Fiordaliso, Elisabetta Maria; Sharafutdinov, Irek; Carvalho, Hudson W. P.; Grunwaldt, Jan-D.; Hansen, Thomas Willum; Chorkendorff, Ib; Wagner, Jakob Birkedal; Damsgaard, Christian Danvad.

In: A C S Catalysis, Vol. 5, No. 10, 2015, p. 5827-5836.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Intermetallic GaPd2 Nanoparticles on SiO2 for Low-Pressure CO2 Hydrogenation to Methanol

T2 - Catalytic Performance and In Situ Characterization

AU - Fiordaliso, Elisabetta Maria

AU - Sharafutdinov, Irek

AU - Carvalho, Hudson W. P.

AU - Grunwaldt, Jan-D.

AU - Hansen, Thomas Willum

AU - Chorkendorff, Ib

AU - Wagner, Jakob Birkedal

AU - Damsgaard, Christian Danvad

PY - 2015

Y1 - 2015

N2 - A nanodispersed intermetallic GaPd2/SiO2 catalyst is prepared by simple impregnation of industrially relevant high-surface-area SiO2 with Pd and Ga nitrates, followed by drying, calcination, and reduction in hydrogen. The catalyst is tested for CO2 hydrogenation to methanol at ambient pressure, revealing that the intrinsic activity of the GaPd2/SiO2 is higher than that of the conventional Cu/ZnO/Al2O3, while the production of the undesired CO is lower. A combination of complementary in situ and ex situ techniques are used to investigate the GaPd2/SiO2 catalyst. In situ X-ray diffraction and in situ extended X-ray absorption fine structure spectroscopy show that the GaPd2 intermetallic phase is formed upon activation of the catalyst via reduction and remains stable during CO2 hydrogenation. Identical location-transmission electron microscopy images acquired ex situ (i.e., micrographs of exactly the same catalyst area recorded at the different steps of activation and reaction procedure) show that nanoparticle size and dispersion are defined upon calcination with no significant changes observed after reduction and methanol synthesis. Similar conclusions can be drawn from electron diffraction patterns and images acquired using environmental TEM (ETEM), indicating that ETEM results are representative for the catalyst treated at ambient pressure. The chemical composition and the crystalline structure of the nanoparticles are identified by scanning TEM energy dispersive X-ray spectroscopy, selected area electron diffraction, and atomically resolved TEM images.

AB - A nanodispersed intermetallic GaPd2/SiO2 catalyst is prepared by simple impregnation of industrially relevant high-surface-area SiO2 with Pd and Ga nitrates, followed by drying, calcination, and reduction in hydrogen. The catalyst is tested for CO2 hydrogenation to methanol at ambient pressure, revealing that the intrinsic activity of the GaPd2/SiO2 is higher than that of the conventional Cu/ZnO/Al2O3, while the production of the undesired CO is lower. A combination of complementary in situ and ex situ techniques are used to investigate the GaPd2/SiO2 catalyst. In situ X-ray diffraction and in situ extended X-ray absorption fine structure spectroscopy show that the GaPd2 intermetallic phase is formed upon activation of the catalyst via reduction and remains stable during CO2 hydrogenation. Identical location-transmission electron microscopy images acquired ex situ (i.e., micrographs of exactly the same catalyst area recorded at the different steps of activation and reaction procedure) show that nanoparticle size and dispersion are defined upon calcination with no significant changes observed after reduction and methanol synthesis. Similar conclusions can be drawn from electron diffraction patterns and images acquired using environmental TEM (ETEM), indicating that ETEM results are representative for the catalyst treated at ambient pressure. The chemical composition and the crystalline structure of the nanoparticles are identified by scanning TEM energy dispersive X-ray spectroscopy, selected area electron diffraction, and atomically resolved TEM images.

KW - Methanol synthesis

KW - Intermetallics

KW - In situ characterization

KW - XRD

KW - TEM

KW - EXAFS

U2 - 10.1021/acscatal.5b01271

DO - 10.1021/acscatal.5b01271

M3 - Journal article

VL - 5

SP - 5827

EP - 5836

JO - A C S Catalysis

JF - A C S Catalysis

SN - 2155-5435

IS - 10

ER -