Publisher: Elsevier BV

Issue:

License: [{"start"=>{"date-parts"=>[[2026, 11, 1]], "date-time"=>"2026-11-01T00:00:00Z", "timestamp"=>1793491200000}, "content-version"=>"tdm", "delay-in-days"=>0, "URL"=>"https://www.elsevier.com/tdm/userlicense/1.0/"}, {"start"=>{"date-parts"=>[[2026, 11, 1]], "date-time"=>"2026-11-01T00:00:00Z", "timestamp"=>1793491200000}, "content-version"=>"tdm", "delay-in-days"=>0, "URL"=>"https://www.elsevier.com/legal/tdmrep-license"}, {"start"=>{"date-parts"=>[[2026, 9, 18]], "date-time"=>"2026-09-18T00:00:00Z", "timestamp"=>1789689600000}, "content-version"=>"vor", "delay-in-days"=>0, "URL"=>"http://creativecommons.org/licenses/by/4.0/"}]

Publication date(s): 2026/11 (print)

Pages: 117179

Volume: 463 Issue:

Journal: Journal of Catalysis

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The effect of the support on the CO2 hydrogenation to ethanol reaction over KRhFe catalysts supported on different oxides (SiO2, Al2O3, TiO2, TiO2-ZrO2, and SiO2-Al2O3) was investigated through a multi-technique approach combining catalytic tests with extensive physicochemical characterisation, including XAS and operando DRIFTS-MS. H2-TPR, TEM and XAS analyses revealed that non-reducible supports, such as SiO2 and Al2O3, stabilise partially oxidised, well-dispersed Rh and Fe species, while maintaining moderate Rh–Fe interactions. In contrast, reducible supports like TiO2 and TiO2-ZrO2 facilitate the reduction of RhOx and FeOx species. This translates into markedly different catalytic behaviours: SiO2 and Al2O3-supported catalysts exhibited enhanced selectivity towards ethanol, whereas TiO2 and TiO2-ZrO2-supported catalysts showed higher CO2 conversion, predominantly yielding CO and CH4. Operando DRIFTS-MS results further revealed plausible support-dependent surface intermediates and reaction pathways. The SiO2-supported catalyst appears to mainly follow a CO-mediated pathway, while the Al2O3-supported catalyst exhibited intense formate-related features, suggesting the participation of formate/methoxy intermediates in oxygenate formation. In contrast, TiO2 promoted RWGS and methanation reactions, limiting C–C coupling. Finally, the incorporation of ZrO2 into the support (TiO2-ZrO2) improved the formation of oxygenates compared to TiO2 alone, likely due to enhanced stabilisation of adsorbed CO species and their coupling with methoxy intermediates. Overall, these results underscore the critical role of metal–support interactions in governing the selectivity between C1 products and oxygenates during high-pressure CO2 hydrogenation.

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