Kim, Dong Ho Oh, Sang-Ho Ha, Heon Phil Joo, Young-Chang Kim, Jongsik 2024-01-19T10:02:38Z 2024-01-19T10:02:38Z 2023-02-10 2023-03 0169-4332 https://pubs.kist.re.kr/handle/201004/113969 CO generates CO2, a feedstock of chemicals including alcohols, alkenes, etc., through exothermic oxidation/ water-gas shift (WGS) on CuO-CeO2 interfaces. However, CO oxidation/WGS with wet, low-temperature gases have been partially explored with regard to surface dynamics, rate laws, rate-determining steps, and catalytic consequences. This study clarifies the aforementioned conundrums via control runs and kinetic assessments. Two CuO-CeO2 interfaces were engineered to possess comparable quantities of CO/H2O-accessible Cu+/2+ species or O2/H2O-accessible mobile (OM), labile (OL), and vacant oxygens, yet, provide distinct binding strengths with CO (ECO), OM (EOM), and H2O (EH2O) alongside with dissimilar H2O-accessible surface areas (SH2O). 18O2-labelling control runs and energy barriers (EBARRIER) of the CuO-CeO2 interfaces corroborated that OM migration outweighed OL migration as the rate-determining step for CO oxidation. The EBARRIER/SH2O values of the CuO-CeO2 interfaces demonstrated that H2O scission overrode CO2 evolution as the rate-determining step for the WGS. CO oxidation competed with yet outperformed WGS in converting CO using wet, low-temperature gases, highlighting the importance of lowering the ECO/EOM values in boost OM migration on CuO-CeO2 interfaces and reducing their EH2O values for hindering WGS. These findings can promote the low-temperature CO transformation performance maximum-obtainable on CuO-CeO2 interfaces. English Elsevier BV Unravelling rate-determining step and consequence of O2-or H2O-assisted, wet CO transformation on catalytic CuO-CeO2 domains via interfacial engineering Article 10.1016/j.apsusc.2022.156099 1 Applied Surface Science, v.614 Applied Surface Science 614 N scie scopus 000912105800001 2-s2.0-85144600195 Chemistry, Physical Materials Science, Coatings & Films Physics, Applied Physics, Condensed Matter Chemistry Materials Science Physics Article GAS SHIFT REACTION METAL-ORGANIC FRAMEWORK HIGH CO2-OVER-N-2 SELECTIVITY PREFERENTIAL OXIDATION LOW-TEMPERATURE COPPER-OXIDE CUO/CEO2 CATALYSTS CARBON-DIOXIDE FLUE-GAS H-2-RICH STREAMS CO oxidation Interfacial engineering Rate-determining step Wet low-temperature gas