Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO                         2                          catalysts

P. M. Yeletsky; T. R. Reina; O. A. Bulavchenko; A. A. Saraev; E. Yu Gerasimov; O. O. Zaikina; J. M. Bermúdez; P. Arcelus-Arrillaga; V. A. Yakovlev; M. Millan

doi:10.1016/j.cattod.2018.10.019

Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO ₂ catalysts

P. M. Yeletsky, T. R. Reina, O. A. Bulavchenko, A. A. Saraev, E. Yu Gerasimov, O. O. Zaikina, J. M. Bermúdez, P. Arcelus-Arrillaga, V. A. Yakovlev^*, M. Millan

^*Corresponding author for this work

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

24 Scopus citations

Abstract

A series of NiMo/SiO ₂ catalysts was synthesized by sol-gel method for heavy oil upgrading in supercritical water (SCW). Phenanthrene was used as substrate as it represents polyaromatic structures present in asphaltenes. No phenanthrene conversion was observed in a blank (non‐catalytic) experiment. However, phenanthrene conversions up to 24% after 1 h of reaction in SCW at 425 °C and 230 bar were observed in the presence of NiMo/SiO ₂ , underlining the role of the catalysts in the process. Conversion was found to be dependent mainly on Ni content and the Ni/Mo ratio in the catalysts. The liquid products obtained are thought to be the result of both oxidation and hydrogenation processes. Characterization of the fresh and spent catalysts using X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) was performed. It was revealed that catalysts are not completely stable in SCW, showing that NiMo intermetallic compounds formed the initial catalysts were decomposed, Mo ⁰ and Ni ⁰ were oxidised and the latter formed Ni ₂ SiO ₄ . In addition, MoO ₂ phase domain size in the catalysts increased and the surface of the spent catalysts appeared to be enriched with Ni and depleted with Mo.

Original language	English
Pages (from-to)	197-205
Number of pages	9
Journal	Catalysis Today
Volume	329
DOIs	https://doi.org/10.1016/j.cattod.2018.10.019
State	Published - 1 Jun 2019
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2018

Keywords

NiMo/SiO
PAHs
Partial oxidation
Phenanthrene
Supercritical water

ASJC Scopus subject areas

Catalysis
General Chemistry

Access to Document

10.1016/j.cattod.2018.10.019

Cite this

Yeletsky, P. M., Reina, T. R., Bulavchenko, O. A., Saraev, A. A., Gerasimov, E. Y., Zaikina, O. O., Bermúdez, J. M., Arcelus-Arrillaga, P., Yakovlev, V. A., & Millan, M. (2019). Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO ₂ catalysts. Catalysis Today, 329, 197-205. https://doi.org/10.1016/j.cattod.2018.10.019

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title = "Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO 2 catalysts",

abstract = " A series of NiMo/SiO 2 catalysts was synthesized by sol-gel method for heavy oil upgrading in supercritical water (SCW). Phenanthrene was used as substrate as it represents polyaromatic structures present in asphaltenes. No phenanthrene conversion was observed in a blank (non‐catalytic) experiment. However, phenanthrene conversions up to 24\% after 1 h of reaction in SCW at 425 °C and 230 bar were observed in the presence of NiMo/SiO 2 , underlining the role of the catalysts in the process. Conversion was found to be dependent mainly on Ni content and the Ni/Mo ratio in the catalysts. The liquid products obtained are thought to be the result of both oxidation and hydrogenation processes. Characterization of the fresh and spent catalysts using X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) was performed. It was revealed that catalysts are not completely stable in SCW, showing that NiMo intermetallic compounds formed the initial catalysts were decomposed, Mo 0 and Ni 0 were oxidised and the latter formed Ni 2 SiO 4 . In addition, MoO 2 phase domain size in the catalysts increased and the surface of the spent catalysts appeared to be enriched with Ni and depleted with Mo.",

keywords = "NiMo/SiO, PAHs, Partial oxidation, Phenanthrene, Supercritical water",

author = "Yeletsky, \{P. M.\} and Reina, \{T. R.\} and Bulavchenko, \{O. A.\} and Saraev, \{A. A.\} and Gerasimov, \{E. Yu\} and Zaikina, \{O. O.\} and Berm{\'u}dez, \{J. M.\} and P. Arcelus-Arrillaga and Yakovlev, \{V. A.\} and M. Millan",

note = "Publisher Copyright: {\textcopyright} 2018",

year = "2019",

month = jun,

day = "1",

doi = "10.1016/j.cattod.2018.10.019",

language = "English",

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pages = "197--205",

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Yeletsky, PM, Reina, TR, Bulavchenko, OA, Saraev, AA, Gerasimov, EY, Zaikina, OO, Bermúdez, JM, Arcelus-Arrillaga, P, Yakovlev, VA & Millan, M 2019, 'Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO ₂ catalysts', Catalysis Today, vol. 329, pp. 197-205. https://doi.org/10.1016/j.cattod.2018.10.019

TY - JOUR

T1 - Phenanthrene catalytic cracking in supercritical water

T2 - effect of the reaction medium on NiMo/SiO 2 catalysts

AU - Yeletsky, P. M.

AU - Reina, T. R.

AU - Bulavchenko, O. A.

AU - Saraev, A. A.

AU - Gerasimov, E. Yu

AU - Zaikina, O. O.

AU - Bermúdez, J. M.

AU - Arcelus-Arrillaga, P.

AU - Yakovlev, V. A.

AU - Millan, M.

PY - 2019/6/1

Y1 - 2019/6/1

N2 - A series of NiMo/SiO 2 catalysts was synthesized by sol-gel method for heavy oil upgrading in supercritical water (SCW). Phenanthrene was used as substrate as it represents polyaromatic structures present in asphaltenes. No phenanthrene conversion was observed in a blank (non‐catalytic) experiment. However, phenanthrene conversions up to 24% after 1 h of reaction in SCW at 425 °C and 230 bar were observed in the presence of NiMo/SiO 2 , underlining the role of the catalysts in the process. Conversion was found to be dependent mainly on Ni content and the Ni/Mo ratio in the catalysts. The liquid products obtained are thought to be the result of both oxidation and hydrogenation processes. Characterization of the fresh and spent catalysts using X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) was performed. It was revealed that catalysts are not completely stable in SCW, showing that NiMo intermetallic compounds formed the initial catalysts were decomposed, Mo 0 and Ni 0 were oxidised and the latter formed Ni 2 SiO 4 . In addition, MoO 2 phase domain size in the catalysts increased and the surface of the spent catalysts appeared to be enriched with Ni and depleted with Mo.

AB - A series of NiMo/SiO 2 catalysts was synthesized by sol-gel method for heavy oil upgrading in supercritical water (SCW). Phenanthrene was used as substrate as it represents polyaromatic structures present in asphaltenes. No phenanthrene conversion was observed in a blank (non‐catalytic) experiment. However, phenanthrene conversions up to 24% after 1 h of reaction in SCW at 425 °C and 230 bar were observed in the presence of NiMo/SiO 2 , underlining the role of the catalysts in the process. Conversion was found to be dependent mainly on Ni content and the Ni/Mo ratio in the catalysts. The liquid products obtained are thought to be the result of both oxidation and hydrogenation processes. Characterization of the fresh and spent catalysts using X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) was performed. It was revealed that catalysts are not completely stable in SCW, showing that NiMo intermetallic compounds formed the initial catalysts were decomposed, Mo 0 and Ni 0 were oxidised and the latter formed Ni 2 SiO 4 . In addition, MoO 2 phase domain size in the catalysts increased and the surface of the spent catalysts appeared to be enriched with Ni and depleted with Mo.

KW - NiMo/SiO

KW - PAHs

KW - Partial oxidation

KW - Phenanthrene

KW - Supercritical water

UR - https://www.scopus.com/pages/publications/85056422230

U2 - 10.1016/j.cattod.2018.10.019

DO - 10.1016/j.cattod.2018.10.019

M3 - Article

AN - SCOPUS:85056422230

SN - 0920-5861

VL - 329

SP - 197

EP - 205

JO - Catalysis Today

JF - Catalysis Today

ER -

Phenanthrene catalytic cracking in supercritical water: effect of the reaction medium on NiMo/SiO 2 catalysts