期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 21, 页码 9131-9137出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c02109
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资金
- U.S. Department of Energy (U.S. DOE), Office of Science and Office of Basic Energy Sciences [DE-SC0012704]
- U.S. DOE [DE-AC02-06CH11357]
- European Union's Horizon 2020 research and innovation program under Marie Sklodowska-Curie Grant [832121]
- PRACE aislb
- MINECO [CTQ201571823-R]
- MICINN-Spain [RTI2018-101604-B-I00]
The clean activation of methane at low temperatures remains an eminent challenge and a field of competitive research. In particular, on late transition metal surfaces such as Pt(111) or Ni(111), higher temperatures are necessary to activate the hydrocarbon molecule, but a massive deposition of carbon makes the metal surface useless for catalytic activity. However, on very low-loaded M/CeO2 (M = Pt, Ni, or Co) surfaces, the dissociation of methane occurs at room temperature, which is unexpected considering simple linear scaling relationships. This intriguing phenomenon has been studied using a combination of experimental techniques (ambient-pressure X-ray photoelectron spectroscopy, time-resolved X-ray diffraction, and X-ray absorption spectroscopy) and density functional theory-based calculations. The experimental and theoretical studies show that the size and morphology of the supported nanoparticles together with strong metal-support interactions are behind the deviations from the scaling relations. These findings point toward a possible strategy for circumventing scaling relations, producing active and stable catalysts that can be employed for methane activation and conversion.
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