DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO2 hydrogenation over Au/γ-Al2O3

Ke Wang; Shibo Shao; Yanrong Liu; Mengyu Cao; Jialin Yu; Cher Hon Lau; Ying Zheng; Xianfeng Fan

doi:10.1016/j.apcatb.2023.122531

DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO₂ hydrogenation over Au/γ-Al₂O₃

Ke Wang, Shibo Shao, Yanrong Liu, Mengyu Cao, Jialin Yu, Cher Hon Lau, Ying Zheng, Xianfeng Fan^*

^*Corresponding author for this work

School of Engineering

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

Abstract

The localized plasmon resonance (LSPR) is recognized as an effective way to convert incident light energy and significantly boost the catalytic reaction. However, a comprehensive understanding of the plasmon-thermo coupling mechanism is still lacking. To address this knowledge gap, we investigate reaction pathway and plasmonic enhancement mechanism of the photo-thermo coupled catalytic reverse water gas shift (RWGS) reactions over Au/γ-Al₂O₃. The results indicate that both formate and carboxyl pathways contribute to the overall reaction. The m-formate pathway is suggested as the main reaction mechanism at low reaction temperature over small Au NPs. Spectro-kinetics and theoretical calculation analyses indicate that the plasmonic energy preferentially transfers to HCOO* via a combination of hot electron and resonance energy transfer mechanisms. The plasmonic energy facilitates the dehydration of HCOO* to CO, which is the rate-determining step (RDS) of the overall RWGS reaction.

Original language	English
Article number	122531
Journal	Applied Catalysis B: Environmental
Volume	328
Early online date	24 Feb 2023
DOIs	https://doi.org/10.1016/j.apcatb.2023.122531
Publication status	Published - 5 Jul 2023

Keywords / Materials (for Non-textual outputs)

CO reduction
In-situ DRIFTS-MS
Localized surface plasmon resonance (LSPR)
Photo-thermo coupling mechanism
Reverse water gas shift (RWGS) reaction

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10.1016/j.apcatb.2023.122531Licence: Creative Commons: Attribution (CC-BY)

https://www.sciencedirect.com/science/article/pii/S0926337323001741Licence: Creative Commons: Attribution (CC-BY)

Cite this

@article{d39bcdd58cfe424ab19b9e9b84d45a93,

title = "DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO2 hydrogenation over Au/γ-Al2O3",

abstract = "The localized plasmon resonance (LSPR) is recognized as an effective way to convert incident light energy and significantly boost the catalytic reaction. However, a comprehensive understanding of the plasmon-thermo coupling mechanism is still lacking. To address this knowledge gap, we investigate reaction pathway and plasmonic enhancement mechanism of the photo-thermo coupled catalytic reverse water gas shift (RWGS) reactions over Au/γ-Al2O3. The results indicate that both formate and carboxyl pathways contribute to the overall reaction. The m-formate pathway is suggested as the main reaction mechanism at low reaction temperature over small Au NPs. Spectro-kinetics and theoretical calculation analyses indicate that the plasmonic energy preferentially transfers to HCOO* via a combination of hot electron and resonance energy transfer mechanisms. The plasmonic energy facilitates the dehydration of HCOO* to CO, which is the rate-determining step (RDS) of the overall RWGS reaction.",

keywords = "CO reduction, In-situ DRIFTS-MS, Localized surface plasmon resonance (LSPR), Photo-thermo coupling mechanism, Reverse water gas shift (RWGS) reaction",

author = "Ke Wang and Shibo Shao and Yanrong Liu and Mengyu Cao and Jialin Yu and Lau, \{Cher Hon\} and Ying Zheng and Xianfeng Fan",

note = "Funding Information: The authors thank the financial supports from the Innovation Academy for Green Manufacture, Chinese Academy of Sciences ( IAGM2022D12 ), the National Natural Science Foundation of China ( 22208348 , 22278402 ), the UK research council EPSRC ( EP/V041665/1 ) and the school of engineering, the University of Edinburgh. Dr. Laetitia Pichevin from the school of geoscience, the University of Edinburgh is much appreciated for the assistance of ICP-OES tests. Dr. David Miller from the school of chemistry, the University of St. Andrews is appreciated for the help on HAADF-STEM characterizations. The authors thank the technical helps from Mr. Fergus Dingwall on lab works. This work has made use of the resources provided by the Edinburgh Compute and Data Facility (ECDF) (http://www.ecdf.ed.ac.uk/) and Compute Canada (www.computecanada.ca). Sincerely appreciate Prof. Suojiang Zhang (IPE, CAS) for his careful academic guidance and great support. ",

year = "2023",

month = jul,

day = "5",

doi = "10.1016/j.apcatb.2023.122531",

language = "English",

volume = "328",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

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TY - JOUR

T1 - DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO2 hydrogenation over Au/γ-Al2O3

AU - Wang, Ke

AU - Shao, Shibo

AU - Liu, Yanrong

AU - Cao, Mengyu

AU - Yu, Jialin

AU - Lau, Cher Hon

AU - Zheng, Ying

AU - Fan, Xianfeng

N1 - Funding Information: The authors thank the financial supports from the Innovation Academy for Green Manufacture, Chinese Academy of Sciences ( IAGM2022D12 ), the National Natural Science Foundation of China ( 22208348 , 22278402 ), the UK research council EPSRC ( EP/V041665/1 ) and the school of engineering, the University of Edinburgh. Dr. Laetitia Pichevin from the school of geoscience, the University of Edinburgh is much appreciated for the assistance of ICP-OES tests. Dr. David Miller from the school of chemistry, the University of St. Andrews is appreciated for the help on HAADF-STEM characterizations. The authors thank the technical helps from Mr. Fergus Dingwall on lab works. This work has made use of the resources provided by the Edinburgh Compute and Data Facility (ECDF) (http://www.ecdf.ed.ac.uk/) and Compute Canada (www.computecanada.ca). Sincerely appreciate Prof. Suojiang Zhang (IPE, CAS) for his careful academic guidance and great support.

PY - 2023/7/5

Y1 - 2023/7/5

N2 - The localized plasmon resonance (LSPR) is recognized as an effective way to convert incident light energy and significantly boost the catalytic reaction. However, a comprehensive understanding of the plasmon-thermo coupling mechanism is still lacking. To address this knowledge gap, we investigate reaction pathway and plasmonic enhancement mechanism of the photo-thermo coupled catalytic reverse water gas shift (RWGS) reactions over Au/γ-Al2O3. The results indicate that both formate and carboxyl pathways contribute to the overall reaction. The m-formate pathway is suggested as the main reaction mechanism at low reaction temperature over small Au NPs. Spectro-kinetics and theoretical calculation analyses indicate that the plasmonic energy preferentially transfers to HCOO* via a combination of hot electron and resonance energy transfer mechanisms. The plasmonic energy facilitates the dehydration of HCOO* to CO, which is the rate-determining step (RDS) of the overall RWGS reaction.

AB - The localized plasmon resonance (LSPR) is recognized as an effective way to convert incident light energy and significantly boost the catalytic reaction. However, a comprehensive understanding of the plasmon-thermo coupling mechanism is still lacking. To address this knowledge gap, we investigate reaction pathway and plasmonic enhancement mechanism of the photo-thermo coupled catalytic reverse water gas shift (RWGS) reactions over Au/γ-Al2O3. The results indicate that both formate and carboxyl pathways contribute to the overall reaction. The m-formate pathway is suggested as the main reaction mechanism at low reaction temperature over small Au NPs. Spectro-kinetics and theoretical calculation analyses indicate that the plasmonic energy preferentially transfers to HCOO* via a combination of hot electron and resonance energy transfer mechanisms. The plasmonic energy facilitates the dehydration of HCOO* to CO, which is the rate-determining step (RDS) of the overall RWGS reaction.

KW - CO reduction

KW - In-situ DRIFTS-MS

KW - Localized surface plasmon resonance (LSPR)

KW - Photo-thermo coupling mechanism

KW - Reverse water gas shift (RWGS) reaction

UR - https://www.scopus.com/pages/publications/85149003875

U2 - 10.1016/j.apcatb.2023.122531

DO - 10.1016/j.apcatb.2023.122531

M3 - Article

AN - SCOPUS:85149003875

SN - 0926-3373

VL - 328

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 122531

ER -

DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO₂ hydrogenation over Au/γ-Al₂O₃

Abstract

Keywords / Materials (for Non-textual outputs)

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Heat Accumulation from Renewables with Valid Energy Storage and Transformation - HARVEST

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DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO2 hydrogenation over Au/γ-Al2O3

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Keywords / Materials (for Non-textual outputs)

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Heat Accumulation from Renewables with Valid Energy Storage and Transformation - HARVEST

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DRIFTS-SSITKA-MS investigations on the mechanism of plasmon preferentially enhanced CO₂ hydrogenation over Au/γ-Al₂O₃