Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen

Dingren Ma; Jing Cao; Kairui Liu; Yexing Zhang; Qiwen Liang; Yajing Huang; Xinyi Guan; Lingling Hu; Chun He; Dehua Xia

doi:10.1016/j.apcatb.2023.122578

Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen

Dingren Ma, Jing Cao, Kairui Liu, Yexing Zhang, Qiwen Liang, Yajing Huang, Xinyi Guan, Lingling Hu, Chun He, Dehua Xia

Physical Sciences and Engineering

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

13 Scopus citations

Abstract

Carbon atoms in the interstitial sites of metal nanoparticles have strong influence on heterogeneous catalysis via electronic metal-support interactions (EMSI). Here, the Pt catalysts with interstitial C-Pt EMSI structures were first developed and identified to boost the removal of ozone (O3) and methyl mercaptan (CH3SH). Experimental results showed that the intrinsic activity of the catalysts with low Pt loading (wt%, 0.95 %) was 186 times higher than that of commercial MnO2. This excellent catalytic performance was attributed to dual-site catalytic structures to promote the adsorption/activation of O3 at interstitial C and capture/oxidation of CH3SH at Pt simultaneously. More importantly, the interstitial C sites retained surface atomic oxygen (*O) with excellent reactivity and lowered the energy barrier of C–S bond breakage, thus achieving efficient decomposition of CH3SH into CO2/SO4 2-. This work provides high-performance catalysts and new mechanistic insights for the synergistic control of O3 and CH3SH.

Original language	English (US)
Pages (from-to)	122578
Journal	Applied Catalysis B: Environmental
Volume	329
DOIs	https://doi.org/10.1016/j.apcatb.2023.122578
State	Published - Mar 6 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-03-15
Acknowledgements: This work was supported by the National Natural Science Foundation of China (Nos. 21876212, 21976214, 41603097, 21673086, 52070195), Guangdong Basic and Applied Basic Research Foundation (2022B1515020097, 2019A1515011015, 2021A1515110224), Opening Fund of the State Key Laboratory of Environmental Geochemistry (SKLEG2022221), the Science and Technology Program of Guangzhou (201904010353) and Fundamental Research Funds for the Central Universities, Sun Yat-sen University (13lgjc10, 19lgpy157, 22lgqb21) for financially supporting this work.

ASJC Scopus subject areas

General Environmental Science
Catalysis
Process Chemistry and Technology

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10.1016/j.apcatb.2023.122578

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title = "Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen",

abstract = "Carbon atoms in the interstitial sites of metal nanoparticles have strong influence on heterogeneous catalysis via electronic metal-support interactions (EMSI). Here, the Pt catalysts with interstitial C-Pt EMSI structures were first developed and identified to boost the removal of ozone (O3) and methyl mercaptan (CH3SH). Experimental results showed that the intrinsic activity of the catalysts with low Pt loading (wt%, 0.95 %) was 186 times higher than that of commercial MnO2. This excellent catalytic performance was attributed to dual-site catalytic structures to promote the adsorption/activation of O3 at interstitial C and capture/oxidation of CH3SH at Pt simultaneously. More importantly, the interstitial C sites retained surface atomic oxygen (*O) with excellent reactivity and lowered the energy barrier of C–S bond breakage, thus achieving efficient decomposition of CH3SH into CO2/SO4 2-. This work provides high-performance catalysts and new mechanistic insights for the synergistic control of O3 and CH3SH.",

author = "Dingren Ma and Jing Cao and Kairui Liu and Yexing Zhang and Qiwen Liang and Yajing Huang and Xinyi Guan and Lingling Hu and Chun He and Dehua Xia",

note = "KAUST Repository Item: Exported on 2023-03-15 Acknowledgements: This work was supported by the National Natural Science Foundation of China (Nos. 21876212, 21976214, 41603097, 21673086, 52070195), Guangdong Basic and Applied Basic Research Foundation (2022B1515020097, 2019A1515011015, 2021A1515110224), Opening Fund of the State Key Laboratory of Environmental Geochemistry (SKLEG2022221), the Science and Technology Program of Guangzhou (201904010353) and Fundamental Research Funds for the Central Universities, Sun Yat-sen University (13lgjc10, 19lgpy157, 22lgqb21) for financially supporting this work.",

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doi = "10.1016/j.apcatb.2023.122578",

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T1 - Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen

AU - Ma, Dingren

AU - Cao, Jing

AU - Liu, Kairui

AU - Zhang, Yexing

AU - Liang, Qiwen

AU - Huang, Yajing

AU - Guan, Xinyi

AU - Hu, Lingling

AU - He, Chun

AU - Xia, Dehua

N1 - KAUST Repository Item: Exported on 2023-03-15 Acknowledgements: This work was supported by the National Natural Science Foundation of China (Nos. 21876212, 21976214, 41603097, 21673086, 52070195), Guangdong Basic and Applied Basic Research Foundation (2022B1515020097, 2019A1515011015, 2021A1515110224), Opening Fund of the State Key Laboratory of Environmental Geochemistry (SKLEG2022221), the Science and Technology Program of Guangzhou (201904010353) and Fundamental Research Funds for the Central Universities, Sun Yat-sen University (13lgjc10, 19lgpy157, 22lgqb21) for financially supporting this work.

PY - 2023/3/6

Y1 - 2023/3/6

N2 - Carbon atoms in the interstitial sites of metal nanoparticles have strong influence on heterogeneous catalysis via electronic metal-support interactions (EMSI). Here, the Pt catalysts with interstitial C-Pt EMSI structures were first developed and identified to boost the removal of ozone (O3) and methyl mercaptan (CH3SH). Experimental results showed that the intrinsic activity of the catalysts with low Pt loading (wt%, 0.95 %) was 186 times higher than that of commercial MnO2. This excellent catalytic performance was attributed to dual-site catalytic structures to promote the adsorption/activation of O3 at interstitial C and capture/oxidation of CH3SH at Pt simultaneously. More importantly, the interstitial C sites retained surface atomic oxygen (*O) with excellent reactivity and lowered the energy barrier of C–S bond breakage, thus achieving efficient decomposition of CH3SH into CO2/SO4 2-. This work provides high-performance catalysts and new mechanistic insights for the synergistic control of O3 and CH3SH.

AB - Carbon atoms in the interstitial sites of metal nanoparticles have strong influence on heterogeneous catalysis via electronic metal-support interactions (EMSI). Here, the Pt catalysts with interstitial C-Pt EMSI structures were first developed and identified to boost the removal of ozone (O3) and methyl mercaptan (CH3SH). Experimental results showed that the intrinsic activity of the catalysts with low Pt loading (wt%, 0.95 %) was 186 times higher than that of commercial MnO2. This excellent catalytic performance was attributed to dual-site catalytic structures to promote the adsorption/activation of O3 at interstitial C and capture/oxidation of CH3SH at Pt simultaneously. More importantly, the interstitial C sites retained surface atomic oxygen (*O) with excellent reactivity and lowered the energy barrier of C–S bond breakage, thus achieving efficient decomposition of CH3SH into CO2/SO4 2-. This work provides high-performance catalysts and new mechanistic insights for the synergistic control of O3 and CH3SH.

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SP - 122578

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

ER -

Interstitial carbon-platinum electronic metal-support interaction structure boost synergistic removal of O3 and CH3SH via surface atomic oxygen

Abstract

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