Ji, Seulgi Jeon, Dong Won Choi, Junghyun Cho, Haneol Park, Bo-In Roh, Ilpyo Choi, Hyungil Kim, Chansoo Kim, Jung Kyu Sim, Uk Li, Danlei Ko, Hyunseok Cho, Sung Beom Choi, Heechae 2024-09-19T01:00:25Z 2024-09-19T01:00:25Z 2024-09-19 2024-12 2050-7488 https://pubs.kist.re.kr/handle/201004/150612 Wide band gap metal oxide semiconductor catalysts mostly exhibit very huge variations of catalytic reaction activities and pathways depending on the preparation conditions, unlike metallic catalyst materials. Atomic-scale modeling and ab initio calculations are extremely challenging for metal oxide semiconductor catalysts because of two main reasons: (i) large discrepancies between computational predictions and experiments, (ii) typical cell size limitations in modeling for dilute level doping (<10(20) cm(-3)) cocatalyst size-dependency (diameter >3 nm). In this study, as a new groundbreaking methodology, we used a combination of density functional theory (DFT) calculations and a newly derived analytical model to systematically investigate the mechanisms of catalytic methane (CH4) oxidation activity change of CeO2. The key hypothesis that the catalytic methane oxidation reaction can be followed by the Fermi level change in CeO2 was well demonstrated via comparison with our multi-scale simulation and several literature reports. Our new method was found to give predictions in the catalytic activity of wide band gap semiconductors for variations in defect concentrations and cocatalyst coverage with advanced efficiency and accuracy, overcoming the typical model size limitation and inaccuracy problems of DFT calculations. English Royal Society of Chemistry Overcoming the limitations of atomic-scale simulations on semiconductor catalysis with changing Fermi level and surface treatment Article 10.1039/d4ta03595j 1 Journal of Materials Chemistry A, v.12, no.48, pp.33537 - 33545 Journal of Materials Chemistry A 12 48 33537 33545 N scie scopus 001309574100001 Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Energy & Fuels Materials Science Article PARTIAL OXIDATION METHANE OXIDATION CO OXIDATION METAL-CATALYSTS DOPED CEO2 PERFORMANCE COMBUSTION DEPOSITION STABILITY CLUSTERS