Different reaction mechanisms of ammonia oxidation reaction on Pt/Al2O3 and Pt/CeZrO2 with various Pt states

Mengmeng Sun, Jingying Liu, Chang Song, Yoshito Ogata, Hanbing Rao, Xiaoqing Zhao, Haidi Xu, Yaoqiang Chen

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

NH3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al2O3 and Pt/CeZrO2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal-support interactions. The homogeneously dispersed Pt species over Pt/Al2O3 exposed Pt(111) because of weak metal-support interactions; there even existed an obvious interface between Pt and Al2O3. While obscure even an overlapped interface was observed over Pt/ CeZrO2, resulting in the formation of PtO because of the oxygen migration from CeZrO2 to Pt species (confirmed by CO-FTIR, the cycled H2-TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al2O3, but two kinds of intermediates, N2H4 and HNO, were observed for Pt/CeZrO2. It consequently resulted in the obvious distinction of the NH3-SCO catalytic performance; the light-off temperatures of NH3 over Pt/Al2O3 and Pt/CeZrO2 were 231 and 275 °C, respectively, while the maximum N2 selectivity (65%) was obtained over Pt/CeZrO2, it was obviously better than that over Pt/Al2O3

Original languageEnglish
Pages (from-to)23102-23111
Number of pages10
JournalACS Applied Materials and Interfaces
Volume11
Issue number26
DOIs
Publication statusPublished - Jan 1 2019

Fingerprint

Ammonia
Metals
Oxidation
Carbon Monoxide
Impregnation
Sustainable development
Health
Oxygen
Transmission electron microscopy
Acids
Temperature

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

Different reaction mechanisms of ammonia oxidation reaction on Pt/Al2O3 and Pt/CeZrO2 with various Pt states. / Sun, Mengmeng; Liu, Jingying; Song, Chang; Ogata, Yoshito; Rao, Hanbing; Zhao, Xiaoqing; Xu, Haidi; Chen, Yaoqiang.

In: ACS Applied Materials and Interfaces, Vol. 11, No. 26, 01.01.2019, p. 23102-23111.

Research output: Contribution to journalArticle

Sun, Mengmeng ; Liu, Jingying ; Song, Chang ; Ogata, Yoshito ; Rao, Hanbing ; Zhao, Xiaoqing ; Xu, Haidi ; Chen, Yaoqiang. / Different reaction mechanisms of ammonia oxidation reaction on Pt/Al2O3 and Pt/CeZrO2 with various Pt states. In: ACS Applied Materials and Interfaces. 2019 ; Vol. 11, No. 26. pp. 23102-23111.
@article{d7948905c5664288abdff9d87c8218b8,
title = "Different reaction mechanisms of ammonia oxidation reaction on Pt/Al2O3 and Pt/CeZrO2 with various Pt states",
abstract = "NH3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al2O3 and Pt/CeZrO2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal-support interactions. The homogeneously dispersed Pt species over Pt/Al2O3 exposed Pt(111) because of weak metal-support interactions; there even existed an obvious interface between Pt and Al2O3. While obscure even an overlapped interface was observed over Pt/ CeZrO2, resulting in the formation of PtO because of the oxygen migration from CeZrO2 to Pt species (confirmed by CO-FTIR, the cycled H2-TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al2O3, but two kinds of intermediates, N2H4 and HNO, were observed for Pt/CeZrO2. It consequently resulted in the obvious distinction of the NH3-SCO catalytic performance; the light-off temperatures of NH3 over Pt/Al2O3 and Pt/CeZrO2 were 231 and 275 °C, respectively, while the maximum N2 selectivity (65{\%}) was obtained over Pt/CeZrO2, it was obviously better than that over Pt/Al2O3",
author = "Mengmeng Sun and Jingying Liu and Chang Song and Yoshito Ogata and Hanbing Rao and Xiaoqing Zhao and Haidi Xu and Yaoqiang Chen",
year = "2019",
month = "1",
day = "1",
doi = "10.1021/acsami.9b02128",
language = "English",
volume = "11",
pages = "23102--23111",
journal = "ACS applied materials & interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "26",

}

TY - JOUR

T1 - Different reaction mechanisms of ammonia oxidation reaction on Pt/Al2O3 and Pt/CeZrO2 with various Pt states

AU - Sun, Mengmeng

AU - Liu, Jingying

AU - Song, Chang

AU - Ogata, Yoshito

AU - Rao, Hanbing

AU - Zhao, Xiaoqing

AU - Xu, Haidi

AU - Chen, Yaoqiang

PY - 2019/1/1

Y1 - 2019/1/1

N2 - NH3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al2O3 and Pt/CeZrO2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal-support interactions. The homogeneously dispersed Pt species over Pt/Al2O3 exposed Pt(111) because of weak metal-support interactions; there even existed an obvious interface between Pt and Al2O3. While obscure even an overlapped interface was observed over Pt/ CeZrO2, resulting in the formation of PtO because of the oxygen migration from CeZrO2 to Pt species (confirmed by CO-FTIR, the cycled H2-TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al2O3, but two kinds of intermediates, N2H4 and HNO, were observed for Pt/CeZrO2. It consequently resulted in the obvious distinction of the NH3-SCO catalytic performance; the light-off temperatures of NH3 over Pt/Al2O3 and Pt/CeZrO2 were 231 and 275 °C, respectively, while the maximum N2 selectivity (65%) was obtained over Pt/CeZrO2, it was obviously better than that over Pt/Al2O3

AB - NH3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al2O3 and Pt/CeZrO2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal-support interactions. The homogeneously dispersed Pt species over Pt/Al2O3 exposed Pt(111) because of weak metal-support interactions; there even existed an obvious interface between Pt and Al2O3. While obscure even an overlapped interface was observed over Pt/ CeZrO2, resulting in the formation of PtO because of the oxygen migration from CeZrO2 to Pt species (confirmed by CO-FTIR, the cycled H2-TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al2O3, but two kinds of intermediates, N2H4 and HNO, were observed for Pt/CeZrO2. It consequently resulted in the obvious distinction of the NH3-SCO catalytic performance; the light-off temperatures of NH3 over Pt/Al2O3 and Pt/CeZrO2 were 231 and 275 °C, respectively, while the maximum N2 selectivity (65%) was obtained over Pt/CeZrO2, it was obviously better than that over Pt/Al2O3

UR - http://www.scopus.com/inward/record.url?scp=85069264412&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85069264412&partnerID=8YFLogxK

U2 - 10.1021/acsami.9b02128

DO - 10.1021/acsami.9b02128

M3 - Article

C2 - 31179684

AN - SCOPUS:85069264412

VL - 11

SP - 23102

EP - 23111

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 26

ER -