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

Journal Article · · Surface Science
 [1];  [2];  [3];  [4]
  1. Fundamental Catalysis, Centre for Research and Development (CRD), SABIC, KAUST, (Saudi Arabia)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). CSE Electrochemical Energy Storage Dept.
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  4. Fundamental Catalysis, Centre for Research and Development (CRD), SABIC, KAUST, (Saudi Arabia)
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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 LaAlO3 (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 α-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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1492780
Alternate ID(s):
OSTI ID: 1636121
OSTI ID: 1691474
Report Number(s):
BNL--210937-2019-JAAM
Journal Information:
Surface Science, Journal Name: Surface Science Journal Issue: C Vol. 680; ISSN 0039-6028
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

Figures / Tables (5)

Figure 1(p. 18)figure Figure 1
Figure 2(p. 19)figure Figure 2
Figure 3(p. 21)figure Figure 3
Figure 4(p. 22)figure Figure 4
Figure 5(p. 23)figure Figure 5

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY