Sustaining metal-organic frameworks for water-gas shift catalysis by non-thermal plasma

Shaojun Xu, Sarayute Chansai, Christina Stere, Burapat Inceesungvorn, Alexandre Goguet, Kanlayawat Wangkawong Wangkawong, Rebecca Taylor, Nadeen Al-Janabi, Christopher Hardacre, Philip A Martin, Fan Xiaolei

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Abstract

The limited thermal and water stability of metal-organic frameworks (MOFs) often restricts their applications in conventional catalysis involving thermal treatment and/or use of water. Non-thermal plasma (NTP) is a promising technique that can overcome barriers in conventional catalysis. Here we report an example of NTP-activated water-gas shift reaction (WGSR) over a MOF (HKUST-1). Significantly, the exceptional stability of HKUST-1 has been sustained under NTP activation and in the presence of water, leading to a high specific rate of 8.8 h−1. We found that NTP-induced water dissociation has a two-fold promotion effect in WGSR, facilitating WGSR by supplying OH, and sustaining the stability and hence activity of HKUST-1. In situ characterisation of HKUST-1 revealed the critical role of open Cu sites in the binding of substrate molecules. This study paves the way for utilising MOFs for a wider range of catalysis.
Original languageEnglish
JournalNature Catalysis
Early online date14 Jan 2019
DOIs
Publication statusEarly online date - 14 Jan 2019

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Water gas shift
Catalysis
Gases
Metals
Plasmas
Water
Hot Temperature
Chemical activation
Heat treatment
Molecules
bis(1,3,5-benzenetricarboxylate)tricopper(II)
Substrates
Binding Sites

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Xu, Shaojun ; Chansai, Sarayute ; Stere, Christina ; Inceesungvorn, Burapat ; Goguet, Alexandre ; Wangkawong, Kanlayawat Wangkawong ; Taylor, Rebecca ; Al-Janabi, Nadeen ; Hardacre, Christopher ; Martin, Philip A ; Xiaolei, Fan. / Sustaining metal-organic frameworks for water-gas shift catalysis by non-thermal plasma. In: Nature Catalysis. 2019.
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abstract = "The limited thermal and water stability of metal-organic frameworks (MOFs) often restricts their applications in conventional catalysis involving thermal treatment and/or use of water. Non-thermal plasma (NTP) is a promising technique that can overcome barriers in conventional catalysis. Here we report an example of NTP-activated water-gas shift reaction (WGSR) over a MOF (HKUST-1). Significantly, the exceptional stability of HKUST-1 has been sustained under NTP activation and in the presence of water, leading to a high specific rate of 8.8 h−1. We found that NTP-induced water dissociation has a two-fold promotion effect in WGSR, facilitating WGSR by supplying OH, and sustaining the stability and hence activity of HKUST-1. In situ characterisation of HKUST-1 revealed the critical role of open Cu sites in the binding of substrate molecules. This study paves the way for utilising MOFs for a wider range of catalysis.",
author = "Shaojun Xu and Sarayute Chansai and Christina Stere and Burapat Inceesungvorn and Alexandre Goguet and Wangkawong, {Kanlayawat Wangkawong} and Rebecca Taylor and Nadeen Al-Janabi and Christopher Hardacre and Martin, {Philip A} and Fan Xiaolei",
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Xu, S, Chansai, S, Stere, C, Inceesungvorn, B, Goguet, A, Wangkawong, KW, Taylor, R, Al-Janabi, N, Hardacre, C, Martin, PA & Xiaolei, F 2019, 'Sustaining metal-organic frameworks for water-gas shift catalysis by non-thermal plasma', Nature Catalysis. https://doi.org/10.1038/s41929-018-0206-2

Sustaining metal-organic frameworks for water-gas shift catalysis by non-thermal plasma. / Xu, Shaojun; Chansai, Sarayute; Stere, Christina; Inceesungvorn, Burapat; Goguet, Alexandre; Wangkawong, Kanlayawat Wangkawong; Taylor, Rebecca; Al-Janabi, Nadeen ; Hardacre, Christopher; Martin, Philip A ; Xiaolei, Fan.

In: Nature Catalysis, 14.01.2019.

Research output: Contribution to journalArticle

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AU - Xu, Shaojun

AU - Chansai, Sarayute

AU - Stere, Christina

AU - Inceesungvorn, Burapat

AU - Goguet, Alexandre

AU - Wangkawong, Kanlayawat Wangkawong

AU - Taylor, Rebecca

AU - Al-Janabi, Nadeen

AU - Hardacre, Christopher

AU - Martin, Philip A

AU - Xiaolei, Fan

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AB - The limited thermal and water stability of metal-organic frameworks (MOFs) often restricts their applications in conventional catalysis involving thermal treatment and/or use of water. Non-thermal plasma (NTP) is a promising technique that can overcome barriers in conventional catalysis. Here we report an example of NTP-activated water-gas shift reaction (WGSR) over a MOF (HKUST-1). Significantly, the exceptional stability of HKUST-1 has been sustained under NTP activation and in the presence of water, leading to a high specific rate of 8.8 h−1. We found that NTP-induced water dissociation has a two-fold promotion effect in WGSR, facilitating WGSR by supplying OH, and sustaining the stability and hence activity of HKUST-1. In situ characterisation of HKUST-1 revealed the critical role of open Cu sites in the binding of substrate molecules. This study paves the way for utilising MOFs for a wider range of catalysis.

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