Ethanol steam reforming on rh catalysts: Theoretical and experimental understanding

Jia Zhang; Ziyi Zhong; X. M. Cao; P. Hu; Michael B. Sullivan; Luwei Chen

doi:10.1021/cs400725k

Ethanol steam reforming on rh catalysts: Theoretical and experimental understanding

Jia Zhang^*, Ziyi Zhong, X. M. Cao, P. Hu, Michael B. Sullivan, Luwei Chen

^*Corresponding author for this work

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

41 Scopus citations

Abstract

Through combined theoretical and experimental efforts, the reaction mechanism of ethanol steam reforming on Rh catalysts was studied. The results suggest that acetaldehyde (CH₃CHO) is an important reaction intermediate in the reaction on nanosized Rh catalyst. Our theoretical work suggests that the H-bond effect significantly modifies the ethanol decomposition pathway. The possible reaction pathway on Rh (211) surface is suggested as CH₃CH₂OH → CH₃CH₂O → CH₃CHO → CH₃CO → CH₃ + CO → CH₂ + CO → CH + CO → C + CO, followed by the water gas shift reaction to yield H₂ and CO₂. In addition, we found that the water-gas shift reaction, not the ethanol decomposition, is the bottleneck for the overall ethanol steam reforming process. The CO + OH association is considered the key step, with a sizable energy barrier of 1.31 eV. The present work first discusses the mechanisms and the water effect in ethanol steam reforming reactions on Rh catalyst from both theoretical and experimental standpoints, which may shed light on designing improved catalysts.

Original language	English
Pages (from-to)	448-456
Number of pages	9
Journal	ACS Catalysis
Volume	4
Issue number	2
DOIs	https://doi.org/10.1021/cs400725k
State	Published - 7 Feb 2014
Externally published	Yes

Keywords

DFT calculations
Rh catalyst
ethanol steam reforming
reaction mechanism
real-time GC/MS analysis

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10.1021/cs400725k

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title = "Ethanol steam reforming on rh catalysts: Theoretical and experimental understanding",

abstract = "Through combined theoretical and experimental efforts, the reaction mechanism of ethanol steam reforming on Rh catalysts was studied. The results suggest that acetaldehyde (CH3CHO) is an important reaction intermediate in the reaction on nanosized Rh catalyst. Our theoretical work suggests that the H-bond effect significantly modifies the ethanol decomposition pathway. The possible reaction pathway on Rh (211) surface is suggested as CH3CH2OH → CH3CH2O → CH3CHO → CH3CO → CH3 + CO → CH2 + CO → CH + CO → C + CO, followed by the water gas shift reaction to yield H2 and CO2. In addition, we found that the water-gas shift reaction, not the ethanol decomposition, is the bottleneck for the overall ethanol steam reforming process. The CO + OH association is considered the key step, with a sizable energy barrier of 1.31 eV. The present work first discusses the mechanisms and the water effect in ethanol steam reforming reactions on Rh catalyst from both theoretical and experimental standpoints, which may shed light on designing improved catalysts.",

keywords = "DFT calculations, Rh catalyst, ethanol steam reforming, reaction mechanism, real-time GC/MS analysis",

author = "Jia Zhang and Ziyi Zhong and Cao, {X. M.} and P. Hu and Sullivan, {Michael B.} and Luwei Chen",

year = "2014",

month = feb,

day = "7",

doi = "10.1021/cs400725k",

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TY - JOUR

T1 - Ethanol steam reforming on rh catalysts

T2 - Theoretical and experimental understanding

AU - Zhang, Jia

AU - Zhong, Ziyi

AU - Cao, X. M.

AU - Hu, P.

AU - Sullivan, Michael B.

AU - Chen, Luwei

PY - 2014/2/7

Y1 - 2014/2/7

N2 - Through combined theoretical and experimental efforts, the reaction mechanism of ethanol steam reforming on Rh catalysts was studied. The results suggest that acetaldehyde (CH3CHO) is an important reaction intermediate in the reaction on nanosized Rh catalyst. Our theoretical work suggests that the H-bond effect significantly modifies the ethanol decomposition pathway. The possible reaction pathway on Rh (211) surface is suggested as CH3CH2OH → CH3CH2O → CH3CHO → CH3CO → CH3 + CO → CH2 + CO → CH + CO → C + CO, followed by the water gas shift reaction to yield H2 and CO2. In addition, we found that the water-gas shift reaction, not the ethanol decomposition, is the bottleneck for the overall ethanol steam reforming process. The CO + OH association is considered the key step, with a sizable energy barrier of 1.31 eV. The present work first discusses the mechanisms and the water effect in ethanol steam reforming reactions on Rh catalyst from both theoretical and experimental standpoints, which may shed light on designing improved catalysts.

AB - Through combined theoretical and experimental efforts, the reaction mechanism of ethanol steam reforming on Rh catalysts was studied. The results suggest that acetaldehyde (CH3CHO) is an important reaction intermediate in the reaction on nanosized Rh catalyst. Our theoretical work suggests that the H-bond effect significantly modifies the ethanol decomposition pathway. The possible reaction pathway on Rh (211) surface is suggested as CH3CH2OH → CH3CH2O → CH3CHO → CH3CO → CH3 + CO → CH2 + CO → CH + CO → C + CO, followed by the water gas shift reaction to yield H2 and CO2. In addition, we found that the water-gas shift reaction, not the ethanol decomposition, is the bottleneck for the overall ethanol steam reforming process. The CO + OH association is considered the key step, with a sizable energy barrier of 1.31 eV. The present work first discusses the mechanisms and the water effect in ethanol steam reforming reactions on Rh catalyst from both theoretical and experimental standpoints, which may shed light on designing improved catalysts.

KW - DFT calculations

KW - Rh catalyst

KW - ethanol steam reforming

KW - reaction mechanism

KW - real-time GC/MS analysis

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U2 - 10.1021/cs400725k

DO - 10.1021/cs400725k

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SN - 2155-5435

VL - 4

SP - 448

EP - 456

JO - ACS Catalysis

JF - ACS Catalysis

IS - 2

ER -

Ethanol steam reforming on rh catalysts: Theoretical and experimental understanding

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Keywords

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