On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane

Changyi Jiang; Emily Loisel; David A. Cullen; James A. Dorman; Kerry M. Dooley

doi:10.1016/j.jcat.2020.11.028

On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane

Changyi Jiang, Emily Loisel, David A. Cullen, James A. Dorman, Kerry M. Dooley

Materials MicroAnalysis

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

51 Scopus citations

Abstract

Sulfur and coking tolerance of Ni-based dry reforming catalysts were examined. Catalysts utilizing both Ce/Zr and Ce/La oxide supports, some with additional Co, were tested. Long-term reaction runs were conducted with and without sulfur in the feed. Catalysts were also characterized by STEM, XPS, XAFS and XANES and CO chemisorption. Only catalysts where Co was also present, and supported on the Ce-Zr oxide, were capable of extended sulfur tolerance at >20 ppm sulfur. This tolerance, along with a greatly reduced coking rate, is linked to Co in intimate contact with Ni, the mixture existing as clusters anchored and influenced electronically by the oxide support. The activation of methane takes place on these sites. Larger metal aggregates formed by ripening during reaction appear to be spectators. The measured activation energies for dry reforming suggest that CO₂ activation takes place at the oxide interface, and is a kinetically significant step.

Original language	English
Pages (from-to)	215-229
Number of pages	15
Journal	Journal of Catalysis
Volume	393
DOIs	https://doi.org/10.1016/j.jcat.2020.11.028
State	Published - Jan 2021

Funding

This work was supported by the National Science Foundation (grant number CBET 1510435). The authors would like to thank Drs. Amitava Roy and Orhan Kizilkaya of the LSU Center for Advanced Structures and Microdevices for help with XAS and XPS. Aberration-corrected STEM imaging was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This work was supported by the National Science Foundation (grant number CBET 1510435). The authors would like to thank Drs. Amitava Roy and Orhan Kizilkaya of the LSU Center for Advanced Structures and Microdevices for help with XAS and XPS. Aberration-corrected STEM imaging was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

Funders	Funder number
National Science Foundation	CBET 1510435
Office of Science

Keywords

Cerium-zirconium oxides
Dry reforming
Nickel-cobalt
Sulfur tolerance

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.jcat.2020.11.028

Cite this

@article{34030865768242bf98c74624f816696b,

title = "On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane",

abstract = "Sulfur and coking tolerance of Ni-based dry reforming catalysts were examined. Catalysts utilizing both Ce/Zr and Ce/La oxide supports, some with additional Co, were tested. Long-term reaction runs were conducted with and without sulfur in the feed. Catalysts were also characterized by STEM, XPS, XAFS and XANES and CO chemisorption. Only catalysts where Co was also present, and supported on the Ce-Zr oxide, were capable of extended sulfur tolerance at >20 ppm sulfur. This tolerance, along with a greatly reduced coking rate, is linked to Co in intimate contact with Ni, the mixture existing as clusters anchored and influenced electronically by the oxide support. The activation of methane takes place on these sites. Larger metal aggregates formed by ripening during reaction appear to be spectators. The measured activation energies for dry reforming suggest that CO2 activation takes place at the oxide interface, and is a kinetically significant step.",

keywords = "Cerium-zirconium oxides, Dry reforming, Nickel-cobalt, Sulfur tolerance",

author = "Changyi Jiang and Emily Loisel and Cullen, {David A.} and Dorman, {James A.} and Dooley, {Kerry M.}",

note = "Publisher Copyright: {\textcopyright} 2020 Elsevier Inc.",

year = "2021",

month = jan,

doi = "10.1016/j.jcat.2020.11.028",

language = "English",

volume = "393",

pages = "215--229",

journal = "Journal of Catalysis",

issn = "0021-9517",

publisher = "Elsevier",

}

TY - JOUR

T1 - On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane

AU - Jiang, Changyi

AU - Loisel, Emily

AU - Cullen, David A.

AU - Dorman, James A.

AU - Dooley, Kerry M.

PY - 2021/1

Y1 - 2021/1

N2 - Sulfur and coking tolerance of Ni-based dry reforming catalysts were examined. Catalysts utilizing both Ce/Zr and Ce/La oxide supports, some with additional Co, were tested. Long-term reaction runs were conducted with and without sulfur in the feed. Catalysts were also characterized by STEM, XPS, XAFS and XANES and CO chemisorption. Only catalysts where Co was also present, and supported on the Ce-Zr oxide, were capable of extended sulfur tolerance at >20 ppm sulfur. This tolerance, along with a greatly reduced coking rate, is linked to Co in intimate contact with Ni, the mixture existing as clusters anchored and influenced electronically by the oxide support. The activation of methane takes place on these sites. Larger metal aggregates formed by ripening during reaction appear to be spectators. The measured activation energies for dry reforming suggest that CO2 activation takes place at the oxide interface, and is a kinetically significant step.

AB - Sulfur and coking tolerance of Ni-based dry reforming catalysts were examined. Catalysts utilizing both Ce/Zr and Ce/La oxide supports, some with additional Co, were tested. Long-term reaction runs were conducted with and without sulfur in the feed. Catalysts were also characterized by STEM, XPS, XAFS and XANES and CO chemisorption. Only catalysts where Co was also present, and supported on the Ce-Zr oxide, were capable of extended sulfur tolerance at >20 ppm sulfur. This tolerance, along with a greatly reduced coking rate, is linked to Co in intimate contact with Ni, the mixture existing as clusters anchored and influenced electronically by the oxide support. The activation of methane takes place on these sites. Larger metal aggregates formed by ripening during reaction appear to be spectators. The measured activation energies for dry reforming suggest that CO2 activation takes place at the oxide interface, and is a kinetically significant step.

KW - Cerium-zirconium oxides

KW - Dry reforming

KW - Nickel-cobalt

KW - Sulfur tolerance

UR - http://www.scopus.com/inward/record.url?scp=85098467803&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2020.11.028

DO - 10.1016/j.jcat.2020.11.028

M3 - Article

AN - SCOPUS:85098467803

SN - 0021-9517

VL - 393

SP - 215

EP - 229

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane

Abstract

Funding

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this