Journal
NATURE CATALYSIS
Volume 3, Issue 12, Pages 1034-1043Publisher
NATURE RESEARCH
DOI: 10.1038/s41929-020-00544-3
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Funding
- Australian Research Council (ARC) [FL140100081]
- ARC [DP170102410]
- ARC under the DECRA Fellowship Scheme [DE160100131]
- DOE Office of Science [DE-AC02-06CH11357]
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Although solar irradiation has demonstrated beneficial synergy for catalytic CO2 hydrogenation, it has long been debated as to whether the observed photo-assisted catalytic enhancement has a photo-activation component or is driven solely by the heating effect. Here, we confirm that surface adsorbates play a critical role in photo-assisted CO2 activation. We isolate the rate-determining intermediate species in the photo-assisted Sabatier reaction by in situ isotopic spectroscopy. Specifically, we reveal that photo-activation of the formate adsorbate (HCO2*) offers an eightfold photo-enhancement on NiOx/La2O3@TiO2. Concurrently, the active La2O3@TiO2 support facilitates the adsorption of CO2, which may contribute to the sustained HCO2* formation and conversion. The findings are crucial as they provide surface intermediary insights in the design of catalysts for photo-assisted CO2 conversion. Ultimately, the understanding may unlock the solar-driven hydrogenation catalytic pathway for other reactions involving HCO2* such as the synthesis of methanol.
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