Mechanistic study of non-thermal plasma assisted CO2 hydrogenation over Ru supported on MgAl layered double hydroxide

Shanshan Xu; Sarayute Chansai; Yan Shao; Shaojun Xu; Yi chi Wang; Sarah Haigh; Yibing Mu; Yilai Jiao; Cristina E. Stere; Huanhao Chen; Xiaolei Fan; Christopher Hardacre

doi:10.1016/j.apcatb.2020.118752

Mechanistic study of non-thermal plasma assisted CO₂ hydrogenation over Ru supported on MgAl layered double hydroxide

Shanshan Xu, Sarayute Chansai, Yan Shao, Shaojun Xu, Yi chi Wang, Sarah Haigh, Yibing Mu, Yilai Jiao, Cristina E. Stere, Huanhao Chen, Xiaolei Fan, Christopher Hardacre

Research output: Journal Publication › Article › peer-review

124 Citations (Scopus)

Abstract

Carbon dioxide (CO₂) hydrogenation to value-added molecules is an attractive way to reduce CO₂ emission via upgrading. Herein, non-thermal plasma (NTP) activated CO₂ hydrogenation over Ru/MgAl layered double hydroxide (LDH) catalysts was performed. The catalysis under the NTP conditions enabled significantly higher CO₂ conversions (∼85 %) and CH₄ yield (∼84 %) at relatively low temperatures compared with the conventional thermally activated catalysis. Regarding the catalyst preparation, it was found that the reduction temperature can affect the chemical state of the metal and metal-support interaction significantly, and thus altering the activity of the catalysts in NTP-driven catalytic CO₂ hydrogenation. A kinetic study revealed that the NTP-catalysis has a lower activation energy (at ∼21 kJ mol⁻¹) than that of the thermal catalysis (ca. 82 kJ mol⁻¹), due to the alternative pathways enabled by NTP, which was confirmed by the comparative in situ diffuse reflectance infrared Fourier (DRIFTS) coupled with mass spectrometry (MS) characterisation of the catalytic systems.

Original language	English
Article number	118752
Journal	Applied Catalysis B: Environmental
Volume	268
DOIs	https://doi.org/10.1016/j.apcatb.2020.118752
Publication status	Published - 5 Jul 2020
Externally published	Yes

Keywords

CO hydrogenation
DRIFTS
Non-thermal plasma (NTP)
Ru/MgAl layered double hydroxide (LDH)

ASJC Scopus subject areas

Catalysis
General Environmental Science
Process Chemistry and Technology

UN SDGs

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

Access to Document

10.1016/j.apcatb.2020.118752

Cite this

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title = "Mechanistic study of non-thermal plasma assisted CO2 hydrogenation over Ru supported on MgAl layered double hydroxide",

abstract = "Carbon dioxide (CO2) hydrogenation to value-added molecules is an attractive way to reduce CO2 emission via upgrading. Herein, non-thermal plasma (NTP) activated CO2 hydrogenation over Ru/MgAl layered double hydroxide (LDH) catalysts was performed. The catalysis under the NTP conditions enabled significantly higher CO2 conversions (∼85 %) and CH4 yield (∼84 %) at relatively low temperatures compared with the conventional thermally activated catalysis. Regarding the catalyst preparation, it was found that the reduction temperature can affect the chemical state of the metal and metal-support interaction significantly, and thus altering the activity of the catalysts in NTP-driven catalytic CO2 hydrogenation. A kinetic study revealed that the NTP-catalysis has a lower activation energy (at ∼21 kJ mol−1) than that of the thermal catalysis (ca. 82 kJ mol−1), due to the alternative pathways enabled by NTP, which was confirmed by the comparative in situ diffuse reflectance infrared Fourier (DRIFTS) coupled with mass spectrometry (MS) characterisation of the catalytic systems.",

keywords = "CO hydrogenation, DRIFTS, Non-thermal plasma (NTP), Ru/MgAl layered double hydroxide (LDH)",

author = "Shanshan Xu and Sarayute Chansai and Yan Shao and Shaojun Xu and Wang, {Yi chi} and Sarah Haigh and Yibing Mu and Yilai Jiao and Stere, {Cristina E.} and Huanhao Chen and Xiaolei Fan and Christopher Hardacre",

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year = "2020",

month = jul,

day = "5",

doi = "10.1016/j.apcatb.2020.118752",

language = "English",

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T1 - Mechanistic study of non-thermal plasma assisted CO2 hydrogenation over Ru supported on MgAl layered double hydroxide

AU - Xu, Shanshan

AU - Chansai, Sarayute

AU - Shao, Yan

AU - Xu, Shaojun

AU - Wang, Yi chi

AU - Haigh, Sarah

AU - Mu, Yibing

AU - Jiao, Yilai

AU - Stere, Cristina E.

AU - Chen, Huanhao

AU - Fan, Xiaolei

AU - Hardacre, Christopher

PY - 2020/7/5

Y1 - 2020/7/5

N2 - Carbon dioxide (CO2) hydrogenation to value-added molecules is an attractive way to reduce CO2 emission via upgrading. Herein, non-thermal plasma (NTP) activated CO2 hydrogenation over Ru/MgAl layered double hydroxide (LDH) catalysts was performed. The catalysis under the NTP conditions enabled significantly higher CO2 conversions (∼85 %) and CH4 yield (∼84 %) at relatively low temperatures compared with the conventional thermally activated catalysis. Regarding the catalyst preparation, it was found that the reduction temperature can affect the chemical state of the metal and metal-support interaction significantly, and thus altering the activity of the catalysts in NTP-driven catalytic CO2 hydrogenation. A kinetic study revealed that the NTP-catalysis has a lower activation energy (at ∼21 kJ mol−1) than that of the thermal catalysis (ca. 82 kJ mol−1), due to the alternative pathways enabled by NTP, which was confirmed by the comparative in situ diffuse reflectance infrared Fourier (DRIFTS) coupled with mass spectrometry (MS) characterisation of the catalytic systems.

AB - Carbon dioxide (CO2) hydrogenation to value-added molecules is an attractive way to reduce CO2 emission via upgrading. Herein, non-thermal plasma (NTP) activated CO2 hydrogenation over Ru/MgAl layered double hydroxide (LDH) catalysts was performed. The catalysis under the NTP conditions enabled significantly higher CO2 conversions (∼85 %) and CH4 yield (∼84 %) at relatively low temperatures compared with the conventional thermally activated catalysis. Regarding the catalyst preparation, it was found that the reduction temperature can affect the chemical state of the metal and metal-support interaction significantly, and thus altering the activity of the catalysts in NTP-driven catalytic CO2 hydrogenation. A kinetic study revealed that the NTP-catalysis has a lower activation energy (at ∼21 kJ mol−1) than that of the thermal catalysis (ca. 82 kJ mol−1), due to the alternative pathways enabled by NTP, which was confirmed by the comparative in situ diffuse reflectance infrared Fourier (DRIFTS) coupled with mass spectrometry (MS) characterisation of the catalytic systems.

KW - CO hydrogenation

KW - DRIFTS

KW - Non-thermal plasma (NTP)

KW - Ru/MgAl layered double hydroxide (LDH)

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