Ni-Mn catalysts on silica-modified alumina for CO2 methanation

Wilbert L. Vrijburg, G. Garbarino, Wei Chen, Alexander Parastaev, Alessandro Longo, Evgeny A. Pidko, Emiel J.M. Hensen (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

10 Downloads (Pure)

Abstract

The viability of the Power-to-Gas (PtG) concept is strongly dependent on the development of highly active and stable methanation catalysts obtained from cheap and abundant elements. In this paper, the promotional effect of MnO on Ni catalysts supported on silica-modified γ-Al2O3 (SA) was investigated in CO2 and CO methanation on catalysts with Mn/Ni atomic ratios between 0 and 0.25. Significantly higher methanation rates and CH4 selectivities were obtained for Mn-promoted compositions compared to Ni-only catalysts. The optimal NiMn/SA (Mn/Ni = 0.25) catalyst exhibited improved stability compared with unpromoted Ni/SA at 20 bar. The nature of the catalyst precursor and active catalyst was studied with STEM-EDX, XPS, and X-ray absorption spectroscopy (XAS). Evidence of a mixed Ni-Mn oxide in the catalyst precursor was obtained by EXAFS. EXAFS measurements revealed that the reduced catalyst consisted of metallic Ni particles and small oxidic Mn2+ species. Moreover, Mn addition improved the Ni dispersion and enhanced the Ni2+ reducibility by weakening the interaction between the Ni-oxide precursor and the support. A mechanistic study involving IR spectroscopy and steady-state isotopic (13CO2) transient kinetic analysis (SSITKA) showed that the presence of Mn enhanced CO2 adsorption and activation.
Original languageEnglish
Pages (from-to)358-371
Number of pages14
JournalJournal of Catalysis
Volume382
DOIs
Publication statusPublished - 1 Feb 2020

Fingerprint

methanation
Methanation
Aluminum Oxide
Silicon Dioxide
Alumina
aluminum oxides
Silica
silicon dioxide
catalysts
Catalysts
Oxides
X ray absorption spectroscopy
Carbon Monoxide
oxides
Catalyst supports
Chemical elements
viability
Energy dispersive spectroscopy
Infrared spectroscopy
X ray photoelectron spectroscopy

Keywords

  • CO valorization
  • Manganese promotion
  • Methanation
  • Nickel
  • Power-to-gas

Cite this

@article{10a6413a02ff4894bdb6096389ac1a28,
title = "Ni-Mn catalysts on silica-modified alumina for CO2 methanation",
abstract = "The viability of the Power-to-Gas (PtG) concept is strongly dependent on the development of highly active and stable methanation catalysts obtained from cheap and abundant elements. In this paper, the promotional effect of MnO on Ni catalysts supported on silica-modified γ-Al2O3 (SA) was investigated in CO2 and CO methanation on catalysts with Mn/Ni atomic ratios between 0 and 0.25. Significantly higher methanation rates and CH4 selectivities were obtained for Mn-promoted compositions compared to Ni-only catalysts. The optimal NiMn/SA (Mn/Ni = 0.25) catalyst exhibited improved stability compared with unpromoted Ni/SA at 20 bar. The nature of the catalyst precursor and active catalyst was studied with STEM-EDX, XPS, and X-ray absorption spectroscopy (XAS). Evidence of a mixed Ni-Mn oxide in the catalyst precursor was obtained by EXAFS. EXAFS measurements revealed that the reduced catalyst consisted of metallic Ni particles and small oxidic Mn2+ species. Moreover, Mn addition improved the Ni dispersion and enhanced the Ni2+ reducibility by weakening the interaction between the Ni-oxide precursor and the support. A mechanistic study involving IR spectroscopy and steady-state isotopic (13CO2) transient kinetic analysis (SSITKA) showed that the presence of Mn enhanced CO2 adsorption and activation.",
keywords = "CO valorization, Manganese promotion, Methanation, Nickel, Power-to-gas",
author = "Vrijburg, {Wilbert L.} and G. Garbarino and Wei Chen and Alexander Parastaev and Alessandro Longo and Pidko, {Evgeny A.} and Hensen, {Emiel J.M.}",
year = "2020",
month = "2",
day = "1",
doi = "10.1016/j.jcat.2019.12.026",
language = "English",
volume = "382",
pages = "358--371",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",

}

Ni-Mn catalysts on silica-modified alumina for CO2 methanation. / Vrijburg, Wilbert L.; Garbarino, G.; Chen, Wei; Parastaev, Alexander; Longo, Alessandro; Pidko, Evgeny A.; Hensen, Emiel J.M. (Corresponding author).

In: Journal of Catalysis, Vol. 382, 01.02.2020, p. 358-371.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Ni-Mn catalysts on silica-modified alumina for CO2 methanation

AU - Vrijburg, Wilbert L.

AU - Garbarino, G.

AU - Chen, Wei

AU - Parastaev, Alexander

AU - Longo, Alessandro

AU - Pidko, Evgeny A.

AU - Hensen, Emiel J.M.

PY - 2020/2/1

Y1 - 2020/2/1

N2 - The viability of the Power-to-Gas (PtG) concept is strongly dependent on the development of highly active and stable methanation catalysts obtained from cheap and abundant elements. In this paper, the promotional effect of MnO on Ni catalysts supported on silica-modified γ-Al2O3 (SA) was investigated in CO2 and CO methanation on catalysts with Mn/Ni atomic ratios between 0 and 0.25. Significantly higher methanation rates and CH4 selectivities were obtained for Mn-promoted compositions compared to Ni-only catalysts. The optimal NiMn/SA (Mn/Ni = 0.25) catalyst exhibited improved stability compared with unpromoted Ni/SA at 20 bar. The nature of the catalyst precursor and active catalyst was studied with STEM-EDX, XPS, and X-ray absorption spectroscopy (XAS). Evidence of a mixed Ni-Mn oxide in the catalyst precursor was obtained by EXAFS. EXAFS measurements revealed that the reduced catalyst consisted of metallic Ni particles and small oxidic Mn2+ species. Moreover, Mn addition improved the Ni dispersion and enhanced the Ni2+ reducibility by weakening the interaction between the Ni-oxide precursor and the support. A mechanistic study involving IR spectroscopy and steady-state isotopic (13CO2) transient kinetic analysis (SSITKA) showed that the presence of Mn enhanced CO2 adsorption and activation.

AB - The viability of the Power-to-Gas (PtG) concept is strongly dependent on the development of highly active and stable methanation catalysts obtained from cheap and abundant elements. In this paper, the promotional effect of MnO on Ni catalysts supported on silica-modified γ-Al2O3 (SA) was investigated in CO2 and CO methanation on catalysts with Mn/Ni atomic ratios between 0 and 0.25. Significantly higher methanation rates and CH4 selectivities were obtained for Mn-promoted compositions compared to Ni-only catalysts. The optimal NiMn/SA (Mn/Ni = 0.25) catalyst exhibited improved stability compared with unpromoted Ni/SA at 20 bar. The nature of the catalyst precursor and active catalyst was studied with STEM-EDX, XPS, and X-ray absorption spectroscopy (XAS). Evidence of a mixed Ni-Mn oxide in the catalyst precursor was obtained by EXAFS. EXAFS measurements revealed that the reduced catalyst consisted of metallic Ni particles and small oxidic Mn2+ species. Moreover, Mn addition improved the Ni dispersion and enhanced the Ni2+ reducibility by weakening the interaction between the Ni-oxide precursor and the support. A mechanistic study involving IR spectroscopy and steady-state isotopic (13CO2) transient kinetic analysis (SSITKA) showed that the presence of Mn enhanced CO2 adsorption and activation.

KW - CO valorization

KW - Manganese promotion

KW - Methanation

KW - Nickel

KW - Power-to-gas

UR - http://www.scopus.com/inward/record.url?scp=85077987719&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2019.12.026

DO - 10.1016/j.jcat.2019.12.026

M3 - Article

VL - 382

SP - 358

EP - 371

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

ER -