Browsing by Author "Hardacre, Christopher"

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    Non-thermal plasma catalysis for CO2conversion and catalyst design for the process
    (Bristol : IOP Publ., 2021) Xu, Shanshan; Chen, Huanhao; Hardacre, Christopher; Fan, Xiaolei
    Catalytic conversion of CO2 to renewable chemicals and fuels is a promising approach to mitigate issues associated with climate change and energy supply deficiency. Hybrid non-thermal plasma (NTP) and catalysis systems, that is, NTP catalysis systems, enable the activation of stable CO2 molecules under relatively mild conditions in comparison with conventional thermal catalysis, and are promising for the energy-efficient conversion of CO2. This review presents the state-of-the-art development of NTP catalysis of CO2 conversion, including CO2 splitting and CO2 hydrogenation and reforming, with the focus on mechanistic insights developed forcatalytic CO2 conversion. Additionally, the role of intrinsic catalyst composition and structure in determining the selectivity of CO2 conversion under NTP conditions is also discussed in light of the need for rational design of catalysts for NTP catalysis. Finally, a perspective on future challenges and opportunities in the development of next-generation catalysts for NTP catalysis and the advanced hybrid NTP catalysis process for practical industrial applications are discussed.
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    Unraveling the H2 Promotional Effect on Palladium-Catalyzed CO Oxidation Using a Combination of Temporally and Spatially Resolved Investigations
    (Washington, DC : ACS, 2018) Stewart, Caomhán; Gibson, Emma K.; Morgan, Kevin; Cibin, Giannantonio; Dent, Andrew J.; Hardacre, Christopher; Kondratenko, Evgenii V.; Kondratenko, Vita A.; McManus, Colin; Rogers, Scott; Stere, Cristina E.; Chansai, Sarayute; Wang, Yi-Chi; Haigh, Sarah J.; Wells, Peter P.; Goguet, Alexandre
    The promotional effect of H2 on the oxidation of CO is of topical interest, and there is debate over whether this promotion is due to either thermal or chemical effects. As yet there is no definitive consensus in the literature. Combining spatially resolved mass spectrometry and X-ray absorption spectroscopy (XAS), we observe a specific environment of the active catalyst during CO oxidation, having the same specific local coordination of the Pd in both the absence and presence of H2. In combination with Temporal Analysis of Products (TAP), performed under isothermal conditions, a mechanistic insight into the promotional effect of H2 was found, providing clear evidence of nonthermal effects in the hydrogen-promoted oxidation of carbon monoxide. We have identified that H2 promotes the Langmuir-Hinshelwood mechanism, and we propose this is linked to the increased interaction of O with the Pd surface in the presence of H2. This combination of spatially resolved MS and XAS and TAP studies has provided previously unobserved insights into the nature of this promotional effect.