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• W4221038676 abstract "This study demonstrates a sustainable catalytic CO2 conversion to near 100% CO selectivity at ambient pressure on In2O3. Critically, high CO yield could be observed at the cost of undesired methanation, using a lower than stoichiometric amount of hydrogen in the feed; 1:1 and 1:0.67 CO2:H2 ratios exhibit 98–99.6% CO selectivity with 25–38% CO2 conversion between 773 and 873 K. CO2 and H2 conversion under steady-state conditions at 773–873 K suggests a 1:1 ratio of adsorbed reactants (with 1:0.67 CO2:H2 feed) on the catalyst surface, underscoring the presence of an ideal reactant composition for the reverse water-gas shift reaction, while H2-rich feed compositions show the H2-dominated surface. Surface electronic structure changes, under near-operating conditions, were explored with near ambient pressure photoelectron spectroscopy (NAPPES), and the interesting findings are as follows: (a) A shift in the valence band to lower binding energy, up to 0.6 eV, was observed because of electron filling at high temperatures. (b) An observation of heterogeneous nature of the catalyst surface under NAPPES measurement conditions is attributed to the generation of active oxygen vacancy (Ov) sites, which in turn changes the work function of In2O3. (c) The above changes are found to be reversible, when the reaction was stopped. Vibrational features of the reactant molecules were observed to be broadened in the active temperature window of the catalyst supporting the heterogeneous character of the catalyst surface because of dynamic Ov generation. By optimizing gas hourly space velocity, CO2:H2 ratio, and reaction temperature, exclusive CO selectivity is possible with a H2:CO2 ratio of ∼0.67, which will avoid the product separation stage altogether, while minimizing the expensive H2 in the reactant feed." @default.
• W4221038676 created "2022-04-03" @default.
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• W4221038676 date "2022-03-04" @default.
• W4221038676 modified "2023-10-01" @default.
• W4221038676 title "Sustainable CO₂ Reduction on In₂O₃ with Exclusive CO Selectivity: Catalysis and In Situ Valence Band Photoelectron Spectral Investigations" @default.
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• W4221038676 doi "https://doi.org/10.1021/acssuschemeng.1c07897" @default.
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