High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane

Katharina Mette; Stefanie Kühl; Andrey Tarasov; Marc G. Willinger; Jutta Kröhnert; Sabine Wrabetz; Annette Trunschke; Michael Scherzer; Frank Girgsdies; Hendrik Düdder; Kevin Kähler; Klaus Friedel Ortega; Martin Muhler; Robert Schlögl; Malte Behrens; Thomas Lunkenbein

doi:10.1021/acscatal.6b01683

High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane

Katharina Mette, Stefanie Kühl, Andrey Tarasov, Marc G. Willinger, Jutta Kröhnert, Sabine Wrabetz, Annette Trunschke, Michael Scherzer, Frank Girgsdies, Hendrik Düdder, Kevin Kähler, Klaus Friedel Ortega, Martin Muhler, Robert Schlögl, Malte Behrens, Thomas Lunkenbein

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

116 Scopus citations

Abstract

Dry reforming of methane (DRM) has been studied for many years as an attractive option to produce synthesis gas. However, catalyst deactivation by coking over nonprecious-metal catalysts still remains unresolved. Here, we study the influence of structural and compositional properties of nickel catalysts on the catalytic performance and coking propensity in the DRM. A series of bulk catalysts with different Ni contents was synthesized by calcination of hydrotalcite-like precursors Ni_xMg_0.67-xAl_0.33(OH)₂(CO₃)_0.17·mH₂O prepared by constant-pH coprecipitation. The obtained Ni/MgAl oxide catalysts contain Ni nanoparticles with diameters between 7 and 20 nm. High-resolution transmission electron microscopy (HR-TEM) revealed a nickel aluminate overgrowth on the Ni particles, which could be confirmed by Fourier transform infrared (FTIR) spectroscopy. In particular, catalysts with low Ni contents (5 mol %) exhibit predominantly oxidic surfaces dominated by Ni²⁺ and additionally some isolated Ni⁰ sites. These properties, which are determined by the overgrowth, effectively diminish the formation of coke during the DRM, while the activity is preserved. A large (TEM) and dynamic (microcalorimetry) metallic Ni surface at high Ni contents (50 mol %) causes significant coke formation during the DRM.

Original language	English
Pages (from-to)	7238-7248
Number of pages	11
Journal	ACS Catalysis
Volume	6
Issue number	10
DOIs	https://doi.org/10.1021/acscatal.6b01683
State	Published - 7 Oct 2016
Externally published	Yes

Keywords

FTIR spectroscopy
carbon deposition
dynamic
heterogeneous catalysis
metal-support interaction
microcalorimetry
overgrowth
transmission electron microscopy

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10.1021/acscatal.6b01683

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Mette, K., Kühl, S., Tarasov, A., Willinger, M. G., Kröhnert, J., Wrabetz, S., Trunschke, A., Scherzer, M., Girgsdies, F., Düdder, H., Kähler, K., Ortega, K. F., Muhler, M., Schlögl, R., Behrens, M., & Lunkenbein, T. (2016). High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane. ACS Catalysis, 6(10), 7238-7248. https://doi.org/10.1021/acscatal.6b01683

@article{6dbf8ef735b2492abec7831146803ee9,

title = "High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane",

abstract = "Dry reforming of methane (DRM) has been studied for many years as an attractive option to produce synthesis gas. However, catalyst deactivation by coking over nonprecious-metal catalysts still remains unresolved. Here, we study the influence of structural and compositional properties of nickel catalysts on the catalytic performance and coking propensity in the DRM. A series of bulk catalysts with different Ni contents was synthesized by calcination of hydrotalcite-like precursors NixMg0.67-xAl0.33(OH)2(CO3)0.17·mH2O prepared by constant-pH coprecipitation. The obtained Ni/MgAl oxide catalysts contain Ni nanoparticles with diameters between 7 and 20 nm. High-resolution transmission electron microscopy (HR-TEM) revealed a nickel aluminate overgrowth on the Ni particles, which could be confirmed by Fourier transform infrared (FTIR) spectroscopy. In particular, catalysts with low Ni contents (5 mol %) exhibit predominantly oxidic surfaces dominated by Ni2+ and additionally some isolated Ni0 sites. These properties, which are determined by the overgrowth, effectively diminish the formation of coke during the DRM, while the activity is preserved. A large (TEM) and dynamic (microcalorimetry) metallic Ni surface at high Ni contents (50 mol %) causes significant coke formation during the DRM.",

keywords = "FTIR spectroscopy, carbon deposition, dynamic, heterogeneous catalysis, metal-support interaction, microcalorimetry, overgrowth, transmission electron microscopy",

author = "Katharina Mette and Stefanie K{\"u}hl and Andrey Tarasov and Willinger, {Marc G.} and Jutta Kr{\"o}hnert and Sabine Wrabetz and Annette Trunschke and Michael Scherzer and Frank Girgsdies and Hendrik D{\"u}dder and Kevin K{\"a}hler and Ortega, {Klaus Friedel} and Martin Muhler and Robert Schl{\"o}gl and Malte Behrens and Thomas Lunkenbein",

note = "Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

month = oct,

day = "7",

doi = "10.1021/acscatal.6b01683",

language = "English",

volume = "6",

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Mette, K, Kühl, S, Tarasov, A, Willinger, MG, Kröhnert, J, Wrabetz, S, Trunschke, A, Scherzer, M, Girgsdies, F, Düdder, H, Kähler, K, Ortega, KF, Muhler, M, Schlögl, R, Behrens, M & Lunkenbein, T 2016, 'High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane', ACS Catalysis, vol. 6, no. 10, pp. 7238-7248. https://doi.org/10.1021/acscatal.6b01683

TY - JOUR

T1 - High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane

AU - Mette, Katharina

AU - Kühl, Stefanie

AU - Tarasov, Andrey

AU - Willinger, Marc G.

AU - Kröhnert, Jutta

AU - Wrabetz, Sabine

AU - Trunschke, Annette

AU - Scherzer, Michael

AU - Girgsdies, Frank

AU - Düdder, Hendrik

AU - Kähler, Kevin

AU - Ortega, Klaus Friedel

AU - Muhler, Martin

AU - Schlögl, Robert

AU - Behrens, Malte

AU - Lunkenbein, Thomas

PY - 2016/10/7

Y1 - 2016/10/7

N2 - Dry reforming of methane (DRM) has been studied for many years as an attractive option to produce synthesis gas. However, catalyst deactivation by coking over nonprecious-metal catalysts still remains unresolved. Here, we study the influence of structural and compositional properties of nickel catalysts on the catalytic performance and coking propensity in the DRM. A series of bulk catalysts with different Ni contents was synthesized by calcination of hydrotalcite-like precursors NixMg0.67-xAl0.33(OH)2(CO3)0.17·mH2O prepared by constant-pH coprecipitation. The obtained Ni/MgAl oxide catalysts contain Ni nanoparticles with diameters between 7 and 20 nm. High-resolution transmission electron microscopy (HR-TEM) revealed a nickel aluminate overgrowth on the Ni particles, which could be confirmed by Fourier transform infrared (FTIR) spectroscopy. In particular, catalysts with low Ni contents (5 mol %) exhibit predominantly oxidic surfaces dominated by Ni2+ and additionally some isolated Ni0 sites. These properties, which are determined by the overgrowth, effectively diminish the formation of coke during the DRM, while the activity is preserved. A large (TEM) and dynamic (microcalorimetry) metallic Ni surface at high Ni contents (50 mol %) causes significant coke formation during the DRM.

AB - Dry reforming of methane (DRM) has been studied for many years as an attractive option to produce synthesis gas. However, catalyst deactivation by coking over nonprecious-metal catalysts still remains unresolved. Here, we study the influence of structural and compositional properties of nickel catalysts on the catalytic performance and coking propensity in the DRM. A series of bulk catalysts with different Ni contents was synthesized by calcination of hydrotalcite-like precursors NixMg0.67-xAl0.33(OH)2(CO3)0.17·mH2O prepared by constant-pH coprecipitation. The obtained Ni/MgAl oxide catalysts contain Ni nanoparticles with diameters between 7 and 20 nm. High-resolution transmission electron microscopy (HR-TEM) revealed a nickel aluminate overgrowth on the Ni particles, which could be confirmed by Fourier transform infrared (FTIR) spectroscopy. In particular, catalysts with low Ni contents (5 mol %) exhibit predominantly oxidic surfaces dominated by Ni2+ and additionally some isolated Ni0 sites. These properties, which are determined by the overgrowth, effectively diminish the formation of coke during the DRM, while the activity is preserved. A large (TEM) and dynamic (microcalorimetry) metallic Ni surface at high Ni contents (50 mol %) causes significant coke formation during the DRM.

KW - FTIR spectroscopy

KW - carbon deposition

KW - dynamic

KW - heterogeneous catalysis

KW - metal-support interaction

KW - microcalorimetry

KW - overgrowth

KW - transmission electron microscopy

UR - http://www.scopus.com/inward/record.url?scp=84990944644&partnerID=8YFLogxK

U2 - 10.1021/acscatal.6b01683

DO - 10.1021/acscatal.6b01683

M3 - Article

AN - SCOPUS:84990944644

SN - 2155-5435

VL - 6

SP - 7238

EP - 7248

JO - ACS Catalysis

JF - ACS Catalysis

IS - 10

ER -

High-Temperature Stable Ni Nanoparticles for the Dry Reforming of Methane

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Keywords

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