Mn monolayer modified Rh for syngas-to-ethanol conversion: A first-principles study

Fengyu Li; De En Jiang; Xiao Cheng Zeng; Zhongfang Chen

doi:10.1039/c1nr11121c

Mn monolayer modified Rh for syngas-to-ethanol conversion: A first-principles study

Fengyu Li, De En Jiang, Xiao Cheng Zeng, Zhongfang Chen

Chemistry

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

31 Scopus citations

Abstract

Rh is unique in its ability to convert syngas to ethanol with the help of promoters. We performed systematic first-principles computations to examine the catalytic performance of pure and Mn modified Rh(100) surfaces for ethanol formation from syngas. CO dissociation on the surface as well as CO insertion between the chemisorbed CH ₃ and the surface are the two key steps. The CO dissociation barrier on the Mn monolayer modified Rh(100) surface is remarkably lowered by ∼1.5 eV compared to that on Rh(100). Moreover, the reaction barrier of CO insertion into the chemisorbed CH ₃ group on the Mn monolayer modified Rh(100) surface is 0.34 eV lower than that of methane formation. Thus the present work provides new mechanistic insight into the role of Mn promoters in improving Rh's selectivity to convert syngas to ethanol.

Original language	English (US)
Pages (from-to)	1123-1129
Number of pages	7
Journal	Nanoscale
Volume	4
Issue number	4
DOIs	https://doi.org/10.1039/c1nr11121c
State	Published - Feb 21 2012

ASJC Scopus subject areas

Materials Science(all)

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abstract = "Rh is unique in its ability to convert syngas to ethanol with the help of promoters. We performed systematic first-principles computations to examine the catalytic performance of pure and Mn modified Rh(100) surfaces for ethanol formation from syngas. CO dissociation on the surface as well as CO insertion between the chemisorbed CH 3 and the surface are the two key steps. The CO dissociation barrier on the Mn monolayer modified Rh(100) surface is remarkably lowered by ∼1.5 eV compared to that on Rh(100). Moreover, the reaction barrier of CO insertion into the chemisorbed CH 3 group on the Mn monolayer modified Rh(100) surface is 0.34 eV lower than that of methane formation. Thus the present work provides new mechanistic insight into the role of Mn promoters in improving Rh's selectivity to convert syngas to ethanol.",

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T1 - Mn monolayer modified Rh for syngas-to-ethanol conversion

T2 - A first-principles study

AU - Li, Fengyu

AU - Jiang, De En

AU - Zeng, Xiao Cheng

AU - Chen, Zhongfang

PY - 2012/2/21

Y1 - 2012/2/21

N2 - Rh is unique in its ability to convert syngas to ethanol with the help of promoters. We performed systematic first-principles computations to examine the catalytic performance of pure and Mn modified Rh(100) surfaces for ethanol formation from syngas. CO dissociation on the surface as well as CO insertion between the chemisorbed CH 3 and the surface are the two key steps. The CO dissociation barrier on the Mn monolayer modified Rh(100) surface is remarkably lowered by ∼1.5 eV compared to that on Rh(100). Moreover, the reaction barrier of CO insertion into the chemisorbed CH 3 group on the Mn monolayer modified Rh(100) surface is 0.34 eV lower than that of methane formation. Thus the present work provides new mechanistic insight into the role of Mn promoters in improving Rh's selectivity to convert syngas to ethanol.

AB - Rh is unique in its ability to convert syngas to ethanol with the help of promoters. We performed systematic first-principles computations to examine the catalytic performance of pure and Mn modified Rh(100) surfaces for ethanol formation from syngas. CO dissociation on the surface as well as CO insertion between the chemisorbed CH 3 and the surface are the two key steps. The CO dissociation barrier on the Mn monolayer modified Rh(100) surface is remarkably lowered by ∼1.5 eV compared to that on Rh(100). Moreover, the reaction barrier of CO insertion into the chemisorbed CH 3 group on the Mn monolayer modified Rh(100) surface is 0.34 eV lower than that of methane formation. Thus the present work provides new mechanistic insight into the role of Mn promoters in improving Rh's selectivity to convert syngas to ethanol.

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Mn monolayer modified Rh for syngas-to-ethanol conversion: A first-principles study

Abstract

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