Bimetallic Rh-Fe catalysts for N2O decomposition: Effects of surface structures on catalytic activity

Hao Chen; Qinghua Lu; Chunhai Yi; Bolun Yang; Suitao Qi

doi:10.1039/c7cp08562a

Bimetallic Rh-Fe catalysts for N₂O decomposition: Effects of surface structures on catalytic activity

Hao Chen
, Qinghua Lu
, Chunhai Yi
, Bolun Yang
, Suitao Qi

School of Chemical Engineering and Technology

Xi'an Jiaotong University

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

19 Scopus citations

Abstract

Well-homogenized RhFe alloy nanoparticles and core-shell structured Fe@Rh nanoparticles were highly dispersed on SBA-15 and then applied to N₂O catalytic conversion. Compared to RhFe/SBA-15, Fe@Rh/SBA-15 showed a higher catalytic activity for N₂O decomposition. This is because the Rh layers covering the Fe core were able to protect against oxidization and so Fe@Rh/SBA-15 was prevented from deactivating. DFT calculations were performed to study the reaction mechanism of N₂O decomposition. The rate-determining step, which was found to be the formation of O₂ from adsorbed oxygen atoms on the surfaces of RhFe and Fe@Rh, revealed that O atoms prefer to be adsorbed on exposed Fe atoms on the surface of RhFe rather than that of Fe@Rh. The calculation results indicate that the exposed Fe atoms tend to be oxidized on the surface of RhFe, resulting in the deactivation of RhFe/SBA-15 during the experiment.

Original language	English
Pages (from-to)	5103-5111
Number of pages	9
Journal	Physical Chemistry Chemical Physics
Volume	20
Issue number	7
DOIs	https://doi.org/10.1039/c7cp08562a
State	Published - 2018

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title = "Bimetallic Rh-Fe catalysts for N2O decomposition: Effects of surface structures on catalytic activity",

abstract = "Well-homogenized RhFe alloy nanoparticles and core-shell structured Fe@Rh nanoparticles were highly dispersed on SBA-15 and then applied to N2O catalytic conversion. Compared to RhFe/SBA-15, Fe@Rh/SBA-15 showed a higher catalytic activity for N2O decomposition. This is because the Rh layers covering the Fe core were able to protect against oxidization and so Fe@Rh/SBA-15 was prevented from deactivating. DFT calculations were performed to study the reaction mechanism of N2O decomposition. The rate-determining step, which was found to be the formation of O2 from adsorbed oxygen atoms on the surfaces of RhFe and Fe@Rh, revealed that O atoms prefer to be adsorbed on exposed Fe atoms on the surface of RhFe rather than that of Fe@Rh. The calculation results indicate that the exposed Fe atoms tend to be oxidized on the surface of RhFe, resulting in the deactivation of RhFe/SBA-15 during the experiment.",

author = "Hao Chen and Qinghua Lu and Chunhai Yi and Bolun Yang and Suitao Qi",

note = "Publisher Copyright: {\textcopyright} the Owner Societies 2018.",

year = "2018",

doi = "10.1039/c7cp08562a",

language = "英语",

volume = "20",

pages = "5103--5111",

journal = "Physical Chemistry Chemical Physics",

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TY - JOUR

T1 - Bimetallic Rh-Fe catalysts for N2O decomposition

T2 - Effects of surface structures on catalytic activity

AU - Chen, Hao

AU - Lu, Qinghua

AU - Yi, Chunhai

AU - Yang, Bolun

AU - Qi, Suitao

N1 - Publisher Copyright: © the Owner Societies 2018.

PY - 2018

Y1 - 2018

N2 - Well-homogenized RhFe alloy nanoparticles and core-shell structured Fe@Rh nanoparticles were highly dispersed on SBA-15 and then applied to N2O catalytic conversion. Compared to RhFe/SBA-15, Fe@Rh/SBA-15 showed a higher catalytic activity for N2O decomposition. This is because the Rh layers covering the Fe core were able to protect against oxidization and so Fe@Rh/SBA-15 was prevented from deactivating. DFT calculations were performed to study the reaction mechanism of N2O decomposition. The rate-determining step, which was found to be the formation of O2 from adsorbed oxygen atoms on the surfaces of RhFe and Fe@Rh, revealed that O atoms prefer to be adsorbed on exposed Fe atoms on the surface of RhFe rather than that of Fe@Rh. The calculation results indicate that the exposed Fe atoms tend to be oxidized on the surface of RhFe, resulting in the deactivation of RhFe/SBA-15 during the experiment.

AB - Well-homogenized RhFe alloy nanoparticles and core-shell structured Fe@Rh nanoparticles were highly dispersed on SBA-15 and then applied to N2O catalytic conversion. Compared to RhFe/SBA-15, Fe@Rh/SBA-15 showed a higher catalytic activity for N2O decomposition. This is because the Rh layers covering the Fe core were able to protect against oxidization and so Fe@Rh/SBA-15 was prevented from deactivating. DFT calculations were performed to study the reaction mechanism of N2O decomposition. The rate-determining step, which was found to be the formation of O2 from adsorbed oxygen atoms on the surfaces of RhFe and Fe@Rh, revealed that O atoms prefer to be adsorbed on exposed Fe atoms on the surface of RhFe rather than that of Fe@Rh. The calculation results indicate that the exposed Fe atoms tend to be oxidized on the surface of RhFe, resulting in the deactivation of RhFe/SBA-15 during the experiment.

UR - https://www.scopus.com/pages/publications/85042162353

U2 - 10.1039/c7cp08562a

DO - 10.1039/c7cp08562a

M3 - 文章

C2 - 29392268

AN - SCOPUS:85042162353

SN - 1463-9076

VL - 20

SP - 5103

EP - 5111

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 7

ER -

Bimetallic Rh-Fe catalysts for N₂O decomposition: Effects of surface structures on catalytic activity

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