XPS and NEXAFS study of the reactions of acetic acid and acetaldehyde over UO2(100) thin film

被引:14
作者
Mudiyanselage, K. [1 ]
Burrell, A. K. [2 ]
Senanayake, S. D. [3 ]
Idriss, H. [1 ]
机构
[1] KAUST, SABIC, CRD, Fundamental Catalysis, Thuwal, Saudi Arabia
[2] Argonne Natl Lab, CSE Electrochem Energy Storage Dept, 9700 S Cass Ave, Argonne, IL 60439 USA
[3] Brookhaven Natl Lab, Chem Div, Upton, NY 11973 USA
关键词
UO2(100) thin film; Actinide oxide; Acetic acid XPS (C1s); Acetaldehyde XPS (C1s); NEXAFS C K-edge of acetic acid; NEXAFS C K-edge of acetaldehyde; UO2(111) SINGLE-CRYSTAL; ABSORPTION FINE-STRUCTURE; SURFACE-CHEMISTRY; URANIUM-DIOXIDE; POLYCRYSTALLINE UO2; RUTILE TIO2; ADSORPTION; OXIDES; WATER; ACETONE;
D O I
10.1016/j.susc.2018.10.017
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reactions of two C2 oxygenates, acetaldehyde (CH3CHO) and acetic acid (CH3COOH), over the (100) terminated surface of UO2 thin film are investigated. The UO2 film (ca. 100 nm thick) was prepared on a LaAIO(3) (100) substrate and its reactions were studied by high-resolution synchrotron X-ray photoelectron spectroscopy (XPS - C 1 s, O 1 s, and U 4f) and Near-Edge X-ray Absorption Fine Structure (NEXAFS - C K-edge). Results show a strong interaction of both molecules with the (100) surface at 300 K. Adsorption of acetic acid at 280 K produces acetates. Upon heating their population steadily decreased (XPS C 1 s) and some enolate or ketene-like species (such as CH2 = COO(a)) are formed (NEXAFS). Acetaldehyde primarily adsorbed molecularly at 300 K and subsequent annealing to 480 K led to alpha-H abstraction making enolates upon interaction with surface O anions. No preferential orientation was detected for acetates while some could be seen for adsorbed acetaldehyde (NEXAFS). Results for the adsorption and reactivity of acetic acid and acetaldehyde on UO2(100) are compared with those of UO2(111) reported previously to further probe into possible structure-sensitive reactions of this actinide metal oxide.
引用
收藏
页码:107 / 112
页数:6
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